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Chinese Journal of Catalysis
2025, Vol. 78
Online: 18 November 2025

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Cover: The research group headed by Professor Zheng Gao-Wei at East China University of Science and Technology has developed an engineered imine reductase (IRED) using directed evolution. This mutant exhibits a specific activity exceeding 100 U mg^–1—the highest reported to date for IREDs. Furthermore, an in situ resin-based adsorption system was implemented, effectively mitigating substrate and product inhibition. The optimized process enables efficient and environmentally friendly enzymatic synthesis of pyrrolidines, highlighting the promising application of this engineered IRED and advanced bioprocessing for the production of 2-aryl pyrrolidines. Read more about the article behind the cover on page 144–155.

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Unveiling spatially resolved charge transfer in S-scheme heterojunctions via KPFM Shan Wang, Bei Cheng, Kezhen Qi 2025, 78:  1-3.  DOI: 10.1016/S1872-2067(25)64810-8 Abstract ( 83 )   HTML ( 12 )   PDF (795KB) ( 37 )

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Interfacial Zn-N bond bridges direct S-scheme charge transfer Feiyan Fu, Yunfeng Li 2025, 78:  4-6.  DOI: 10.1016/S1872-2067(25)64809-1 Abstract ( 74 )   HTML ( 9 )   PDF (3830KB) ( 33 )

Reviews

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Discovery and development of cocktail-type catalysis Anton L. Maximov, Mikhail P. Egorov 2025, 78:  7-24.  DOI: 10.1016/S1872-2067(25)64824-8 Abstract ( 65 )   HTML ( 4 )   PDF (2232KB) ( 30 )   Catalysis is a cornerstone of modern chemistry, enabling the development of sustainable processes and the production of essential chemicals. However, a fundamental challenge in catalysis lies in understanding the nature of the catalytic species and active centers, particularly the key mechanistic understanding of homogeneous and heterogeneous systems. This review describes the concept of “cocktail”-type catalysis, demonstrating that catalytic active species are not static but evolve through the interconversion of molecular complexes, clusters, and nanoparticles. By bridging homogeneous and heterogeneous catalysis, this paradigm challenges conventional mechanistic views and initiates discussions for a universal theory of catalysis. The findings highlight the importance of adaptive catalyst behavior, leading to more efficient, selective, and robust catalytic systems. The impact of the “cocktail”-type approach extends beyond fundamental research, offering practical applications in industrial catalysis, green chemistry, and synthetic methodologies. By embracing catalytic dynamics, new opportunities arise for designing next-generation catalysts that are both versatile and highly effective in diverse transformations.

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Refining lignin into aromatic nitrogen-heterocyclic compounds: Sustainable avenue toward value-added chemicals Wentao Su, Shenglong Tian, Huamei Yang, Changzhi Li, Tao Zhang 2025, 78:  25-46.  DOI: 10.1016/S1872-2067(25)64798-X Abstract ( 39 )   HTML ( 2 )   PDF (4789KB) ( 13 )   Lignin is the only largest renewable aromatic resource in nature. Currently, most lignin is underutilized for low-value applications due to the complex structure and recalcitrant chemical properties. Over the past decades, extensive research has been devoted to valorizing lignin into aromatic N-heterocycles in the presence of nitrogen sources. It overcomes the element limitation, expands the products portfolio and would play a momentous role in value-added biorefinery concept. In this review, the latest research progress in the synthesis of N-heterocyclic compounds from lignin, lignin model compounds, and lignin-derived monomers (phenols, aromatic alcohols, aldehydes, ketones, and ethers) is presented. According to the structural characteristics of the products, these achievements are classified by the construction of five-, six-, and seven-membered N-heterocyclic compounds through one-step, multi-step, or one-pot multi-step reactions. Furthermore, the tailor-designed routes and catalytic systems, along with the reaction mechanisms/pathways involved are entirely discussed to elucidate the challenges regarding the structural complexity of lignin, the incompatible catalysis for C-O cleavage and C-N formation, as well as the nitrogen-heterocyclic ring construction. The prospects, future research efforts and process developments for the refining of lignin into aromatic N-heterocyclic compounds are outlined in terms of economy, environmental friendliness, and safety so as to draw some guidelines for lignin valorization.

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The application of photocatalysis and biodegradation synergistic systems in environmental remediation: A review Ruilin Cao, Yuan Pan, Xiansheng Zhang, Xinyi Huang, Teng Li, Sheng Liu, Yunze Wang, Shanqing Tang, Binbin Shao, Zhifeng Liu 2025, 78:  47-74.  DOI: 10.1016/S1872-2067(25)64807-8 Abstract ( 44 )   HTML ( 3 )   PDF (7944KB) ( 12 )   The growing presence of emerging pollutants in the environment has led to a focus on developing new treatment technologies to address the limitations of traditional methods. Recent advancements in combining photocatalysis with biodegradation for pollutant treatment have garnered significant attention. This is due to the rapid and uncontrolled chemical reactions in single photocatalytic processes, which often result in the buildup of harmful by-products and over-oxidation residues. Additionally, relying solely on biodegradation is challenging for breaking down emerging pollutants that possess high concentrations and intricate structures. Therefore, the intimately coupled photocatalysis and biodegradation (ICPB) systems, along with the photocatalytic microbial fuel cells (PMFCs), as a new approach to treat pollutants. These systems combine the benefits of biodegradation and photocatalytic reactions, providing cost-effective, eco-friendly, and sustainable solutions with significant promise. In order to demonstrate the ICPB system and the PMFCs system as rational options for pollutant removal, the mechanisms of pollutant degradation by the two systems have been analyzed in depth, and recent advances in photocatalysts, biofilms, and carriers/configurations in the two systems have been summarized. Furthermore, the practical applications of the ICPB system versus the PMFCs system for pollutant removal are also summarized and highlighted. This review further points out the current limitations, such as photocatalytic materials that are still challenging in terms of commercial viability for practical applications, and looks forward to the prospects of the ICPB system versus the PMFCs system for the treatment of pollutants to promote practical applications.

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Recent advances in graded nanomaterial-based photocatalysts: Principles, designs, and applications Jiale Lv, Hailiang Chu, Chunfeng Shao, Lixian Sun, Graham Dawson, Kai Dai 2025, 78:  75-99.  DOI: 10.1016/S1872-2067(25)64825-X Abstract ( 75 )   HTML ( 2 )   PDF (4040KB) ( 15 )   The rise in global energy demand and environmental pollution highlights the importance of developing efficient and stable photocatalytic materials to address the energy crisis and environmental issues. Graded nanomaterials exhibit significant promise for photocatalysis due to their unique structural advantages, including multi-scale pores, high specific surface area, and optimized electron transport pathways. This review systematically examines the design principles and synthesis methods for hierarchical nanomaterials and their photocatalytic performance. Through modulation of porous structures, hierarchical heterojunctions, and core-shell configurations, graded nanomaterials notably improve light absorption efficiency, carrier separation, and surface reaction activity of photocatalysts. Strategies such as S-scheme heterojunctions and interface engineering further enhance the performance of photocatalysts for CO2 reduction, hydrogen production, and pollutant degradation. In situ characterization techniques offer dynamic insights into the photocatalytic mechanism. This study elucidates how hierarchical structures influence photocatalytic performance, discusses their potential applications in environmental treatment and clean energy, and proposes directions for future design and optimization of photocatalytic materials.

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Future development of single-atom catalysts in portable energy and sensor technologies Tianyou Zhao, Fengming Hu, Meiqi Zhu, Chang-Jie Yang, Xin-Yu Wang, Yong-Zhou Pan, Jiarui Yang, Xia Zhang, Wen-Hao Li, Dingsheng Wang 2025, 78:  100-137.  DOI: 10.1016/S1872-2067(25)64814-5 Abstract ( 53 )   HTML ( 4 )   PDF (5213KB) ( 16 )   With the rapid advancement of portable energy devices and sensor technologies, enhancing their catalytic performance, sensing capabilities, and application reliability has become a critical challenge in the fields of materials and energy science. Single-atom catalysts (SACs), owing to their high atomic utilization, outstanding catalytic activity, and precisely engineered structures enabled by density functional theory and enhanced by artificial intelligence, have shown tremendous potential in advancing portable energy and sensing technologies. While existing reviews predominantly focus on the application of SACs in individual portable devices, systematic discussions on their overall development prospects and challenges within portable energy and sensor fields remain scarce. Therefore, this review comprehensively explores the application potential and recent advancements of SACs in portable zinc-air batteries, proton exchange membrane fuel cells, and sensor technologies. The article highlights the influence of key factors such as material design, structural optimization, and packaging integration on device performance, while also addressing the primary bottlenecks and challenges encountered in current practical applications. Furthermore, it suggests possible future development directions, aiming to offer theoretical insights and engineering guidance for the large-scale deployment of SACs in wearable electronic devices, portable energy systems, and smart sensing technologies.

Communication

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Enantioselective induction by G-quadruplex DNA/hemin in intramolecular cyclopropanation Wenhui Miao, Jingya Hao, Wenqin Zhou, Guoqing Jia, Can Li 2025, 78:  138-143.  DOI: 10.1016/S1872-2067(25)64797-8 Abstract ( 50 )   HTML ( 3 )   PDF (1323KB) ( 20 )   Supporting Information G-quadruplex DNA (G4) can function as a kind of nucleic acid apoenzyme for constructing G4/hemin biocatalyst to mimic the catalytic function of hemoprotein. However, achieving stereoselective control with G4/hemin remains a persistent challenge. Here, we report that a PW17/hemin (PW17: 5’-GGGTAGGGCGGGTTGGG-3’), adopting the 5’-5’ stacked dimeric parallel G4 topology, can realize the enantioselective induction in intramolecular cyclopropanation of allyl diazoacetates with enantioselectivity up to 87% ee. Spectroscopic characterization and catalytic results demonstrate that the relatively open G-quartet of the 3’ terminal in dimeric PW17 contributes a catalytic pocket for hemin accommodation and plays a pivotal role in enantioselective control. This finding expands the unique repertoire of heme enzyme using biological scaffolds from proteins to nucleic acids and resolves the long-standing challenge of stereochemical control in G4/hemin catalysis.

Articles

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Engineering an imine reductase for enhanced activity and reduced substrate inhibition: Asymmetric synthesis of chiral 2-aryl pyrrolidines Xin-Ru Chen, Tian Jin, Chi Zhang, Zhen-Yu Zhu, Xin-Yuan Shen, Qi Chen, Jing Wang, Jian-He Xu, Gao-Wei Zheng 2025, 78:  144-155.  DOI: 10.1016/S1872-2067(25)64767-X Abstract ( 66 )   HTML ( 6 )   PDF (1913KB) ( 31 )   Supporting Information Imine reductases (IREDs) have been extensively used for the imine reduction and reductive amination to access various amines. However, poor activity and severe substrate/product inhibition limit their widespread application in industry. Herein, an engineered IRED from Streptomyces viridochromogenes was developed through four rounds of directed evolution. The engineered SvIRED displayed a significant increase in specific activity to 136.8 U mg−1, the highest reported for an IRED to date. Molecular dynamics simulations elucidated the surge in specific activity during mutations. The best mutant can also catalyse the reductive coupling of aldehyde homologs and primary amines with up to 66.9 U mg−1. Additionally, we established an in-situ product adsorption system using resin, which significantly alleviated substrate/product inhibition and enhanced substrate loading to 100 g L−1. Under optimal conditions, a wide range of chiral 2-aryl-pyrrolidines were successfully produced at high substrate loadings (50-100 g L−1) with enantiomeric excess over 99%. The usefulness of this biocatalytic system was further demonstrated by preparation of pharmaceutically relevant chiral 2-aryl pyrrolidines, particularly the decagram-scale synthesis of the key chiral aticaprant intermediate with 90% isolated yield, >99% ee, and 438 g L−1 d−1 space-time yield.

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Regulating microenvironment of heterogeneous Rh mononuclear complex via sulfur-phosphine co-coordination to enhance the performance of hydroformylation of olefins Siquan Feng, Cunyao Li, Yuxuan Zhou, Xiangen Song, Miao Jiang, HuFei Dai, Shangsheng Song, Benhan Fan, Yutong Cai, Bin Li, Qiao Yuan, Xingju Li, Lei Zhu, Yue Zhang, Weimiao Chen, Tao Liu, Li Yan, Xueqing Gong, Yunjie Ding 2025, 78:  156-169.  DOI: 10.1016/S1872-2067(25)64795-4 Abstract ( 85 )   HTML ( 4 )   PDF (2006KB) ( 42 )   Supporting Information Sulfur was typically regarded as a poison to precious metal complex catalysts in hydroformylation of olefins. However, the combination of sulfur and phosphine may present an intriguing interaction with heterogeneous mononuclear complex due to the difference of their electronegativities, and coordination capabilities. Herein, we report a novel sulfur-phosphine co-coordinated heterogeneous Rh mononuclear complex catalyst (Rh₁/POPs-PPh3&S), which exhibits an unexpected 1.5-2.0 times catalytic activity for hydroformylation of olefins (C3=, C5=-C8=), in comparison with the solely phosphine-coordinated Rh mononuclear complex catalyst (Rh1/POPs-PPh3). In contrast, sulfur coordination alone leads to severe sulfur poisoning with significantly inhibited catalytic performance. Experimental and theoretical analyses reveal that phosphine coordination promotes catalytic activity via its strong electron-donating ability, while sulfur occupies a coordination site and reduces the electronic density of Rh ions. The synergistical coordination of sulfur and phosphine optimizes the electronic density of active Rh ions and decreases the energy barrier of the rate-determining step of olefin insertion, thus enhancing the hydroformylation activity, regioselectivity and stability of Rh₁/POPs-PPh3&S.

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An atom-efficient electrosynthesis strategy for organic halides Yiwei Liu, Xiaoxia Chang, Bingjun Xu 2025, 78:  170-181.  DOI: 10.1016/S1872-2067(25)64796-6 Abstract ( 49 )   HTML ( 1 )   PDF (2692KB) ( 21 )   Supporting Information Existing organic halide synthesis routes typically employ elemental halogens (X2, X = Cl or Br), leading to low atom economy and significant environmental pollution. In this work, we developed an atom efficient electrosynthesis and separation strategy for halogenation reagents — N-chlorosuccinimide (NCS) and N-bromosuccinimide (NBS) — at high current densities. Faradic efficiency (FE) of 91.0% and 81.3% was achieved for NCS and NBS generation on RuOx/TiO2/Ti in a batch cell, respectively. Electrosynthesis of NCS likely involves both heterogeneous catalytic and homogeneous tandem pathways, while NBS is likely formed in a Langmuir-Hinshelwood mechanism with a proton-coupled electron transfer as the rate-determining step. A coupled continuous electrocatalytic synthesis and in situ separation setup was developed for the efficient production of NCS and NBS, which yielded 0.77 g of NCS in 12000 s and 0.81 g of NBS in 15000 s, both with relative purity exceeding 95%. The halogenation of acetone using NCS and NBS enabled gram-scale production of the key intermediate in organic synthesis, 1-halogenacetone, with over 95% recovery of succinimide.

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Computational redesign of a thermostable MHET hydrolase and its role as an endo-PETase in promoting PET depolymerization Xiaomeng Liu, Zehua Chen, Xinyue Liu, Tong Zhu, Jinyuan Sun, Chunli Li, Yinglu Cui, Bian Wu 2025, 78:  182-191.  DOI: 10.1016/S1872-2067(25)64802-9 Abstract ( 43 )   HTML ( 2 )   PDF (1609KB) ( 21 )   Supporting Information Biotechnological strategies for plastic depolymerization and recycling have emerged as transformative approaches to combat the global plastic pollution crisis, aligning with the principles of a sustainable and circular economy. Despite advances in engineering PET hydrolases, the degradation process is frequently compromised by product inhibition and the heterogeneity of final products, thereby obstructing subsequent PET recondensation and impeding the synthesis of high-value derivatives. In this work, we utilized previously devised computational strategies to redesign a thermostable DuraMHETase, achieving an apparent melting temperature of 72 °C in complex with MHET and a 6-fold higher in total turnover number (TTN) toward MHET than the wild-type enzyme at 60 °C. The fused enzyme system composed of DuraMHETase and TurboPETase demonstrated higher efficiency than other PET hydrolases and the separated dual enzyme systems. Furthermore, we identified both exo- and endo-PETase activities in DuraMHETase, whereas the endo- activity was previously unobserved at ambient temperatures. These results expand the functional scope of MHETase beyond mere intermediate hydrolysis, and may provide guidance for the development of more synergistic approaches to plastic biodepolymerization and recycling.

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Reactant-modulated catalytic alcoholysis of polylactic acid from real-life biodegradable plastic waste Chang He, Zhenbo Guo, Zhijun Wang, Yi Ji, Linrui Li, Xin Qiu, Zhuo Liu, Zhaowen Dong, Guangjin Hou, Meng Wang, Fan Zhang 2025, 78:  192-201.  DOI: 10.1016/S1872-2067(25)64811-X Abstract ( 45 )   HTML ( 1 )   PDF (1917KB) ( 9 )   Supporting Information Alcoholysis is one of the most effective methods for recycling polyester plastics. While many researchers claim that both alcohol and polymer reactants are activated simultaneously in the alcoholysis reaction, more reliable experimental evidence is needed to fully understand the process, and the catalytic mechanism remains elusive. To address this issue, we proposed a reactant-modulated catalytic depolymerization strategy involving a pre-mixing of alcohol or polylactic acid (PLA) with an organic base catalyst. Through systematic experimental and theoretical investigations, we have confirmed that different intermediates are formed during pre-mixing the catalyst with PLA or methanol, which can either slow down or accelerate the subsequent alcoholysis reaction. By employing the methanol-modulated depolymerization technique, we successfully achieved PLA alcoholysis at temperatures as low as -40 °C. We further investigated the solubility and reactivity of different polyesters, including PET, PC, PBS, PBAT, PCL, and PLA, revealing an efficient recycling method for PLA. By optimizing reaction conditions in a continuous flow reactor, we recovered 127.3 g of methyl lactate from 100 g of plastic cups in just 4 h at room temperature. These findings greatly improve our grasp of polyester solvolysis processes and create new opportunities within the plastics sector recycling.

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MOF encapsulation derived slow-release oxygen species to enhance the activity and selectivity of methane selective oxidation: A transient DRIFTs Study Ke-Xin Li, Hao Yuan, Ralph T. Yang, Zhun Hu 2025, 78:  202-214.  DOI: 10.1016/S1872-2067(25)64803-0 Abstract ( 32 )   HTML ( 2 )   PDF (2259KB) ( 5 )   Supporting Information The methane selective oxidation was a "holy grail" reaction. However, peroxidation and low selectivity limited the application. Herein, we combined three Au contents with TiO2 in both encapsulation (xAu@TiO2) and surface-loaded (xAu/TiO2) ways by MOF derivation strategy, reported a catalyst 0.5Au@TiO2 exhibited a CH3OH yield of 32.5 μmol·g-1·h-1 and a CH3OH selectivity of 80.6% under catalytic conditions of only CH4, O2, and H2O. Mechanically speaking, the catalytic activity was controlled by both electron-hole separation efficiency and core-shell structure. The interfacial contact between Au nanoparticles and TiO2 in xAu@TiO2 and xAu/TiO2 induced the formation of oxygen vacancies, with 0.5 Au content showing the highest oxygen vacancy concentration. At the same Au content, xAu@TiO2 generated more oxygen vacancies than xAu/TiO2. The oxygen vacancy acted as an effective electron cold trap, which enhanced the photogenerated carrier separation efficiency and thereby improved the catalytic activity. In-situ DRIFTs revealed that the isolated OH (non-hydrogen bond adsorption) were key species for the methane selective oxidation, playing a role in the activation of CH4 to *CH3. However, an overabundance of isolated OH led to severe overoxidation. Fortunately, the core-shell structure over xAu@TiO2 provided a slow-release environment for isolated OH through the intermediate state of *OH (hydrogen bond adsorption) to balance the formation rate and consumption rate of isolated OH, doubling the methanol yield and increasing the > 29% selectivity. These results showed a new strategy for the control of the overoxidation rate via a strategy of MOF encapsulation followed by pyrolytic derivation for methane selective oxidation.

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Channel-passing growth mechanism of coke in ZSM-5 catalyzed methanol-to-hydrocarbons conversion: From molecular structure, spatiotemporal dynamics to catalyst deactivation Nan Wang, Yimo Wu, Jingfeng Han, Yanan Zhang, Li Wang, Yang Yu, Jiaxing Zhang, Hao Xiong, Xiao Chen, Yida Zhou, Hanlixin Wang, Zhaochao Xu, Shutao Xu, Xinwen Guo, Fei Wei, Yingxu Wei, Zhongmin Liu 2025, 78:  215-228.  DOI: 10.1016/S1872-2067(25)64806-6 Abstract ( 37 )   HTML ( 1 )   PDF (5271KB) ( 6 )   Supporting Information Coke formation is the primary cause of zeolite deactivation in industrial catalysis, yet the structural identity, spatial location and molecular routes of polycyclic aromatic hydrocarbons (PAHs) within confined zeolite pores remain elusive. Here, by coupling matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry with multi-dimensional chemical imaging, we unveil a channel-passing growth mechanism for PAHs in ZSM-5 zeolites during methanol conversion through identifying the molecular fingerprints of larger PAHs, pinpointing and visualizing their 3D location and spatiotemporal evolution trajectory with atomic resolution and at both channel and single-crystal scales. Confined aromatic entities cross-link with each other, culminating in multicore PAH chains as the both thermodynamically favorable and kinetically trapped host-guest entanglement wrought and templated by the defined molecular-scale constrained microenvironments of zeolite. The mechanistic concept proves general across both channel- and cage-structured zeolite materials. Our multiscale deactivating model based on the full-picture coke structure-location correlations—spanning atom, molecule, channel/cage and single crystal scales—would shed new light on the intertwined chemical and physical processes in catalyst deactivation. This work not only resolves long-standing puzzles in coke formation but also provides design principles for coke-resistant zeolites. The methods and insights would rekindle interest in confinement effects and host-guest chemistry across broader chemistry fields beyond catalysis and carbon materials.

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Ni-N bonds boost S-scheme charge transfer in NiSe/Cv-C3N5 for efficient water splitting Yan Cao, Lin Ye, Yangchen Yuan, Ruitao Yang, Hui Hong, Jingwen Chen, Jinyi Lu, Entian Cui, Jizhou Jiang 2025, 78:  229-241.  DOI: 10.1016/S1872-2067(25)64832-7 Abstract ( 73 )   HTML ( 1 )   PDF (4770KB) ( 19 )   Supporting Information Constructing heterojunction photocatalysts is a highly effective strategy for achieving overall water splitting, particularly by overcoming the challenge of sluggish electron-hole transport. This study employed a defect-induced in situ growth approach to anchor NiSe onto carbon-vacancy-rich C3N5 (Cv-C3N5), forming interfacial Ni-N bonds. The resulting NiSe/Cv-C3N5 heterojunction exhibited stoichiometric H2 and O2 evolution rates of 1956.1 and 989.1 μmol g-1 h-1, respectively, 8.4 times higher than a counterpart lacking interfacial bonding. Both theoretical calculations and experimental data confirmed that the Ni-N bonds were instrumental in enhancing photocatalytic performance by inducing and reinforcing S-scheme charge transfer. Illumination X-ray photoelectron spectroscopy analysis revealed that a synergistic charge transfer pathway: photoexcited electrons from the NiSe conduction band migrated sequentially to Ni atoms, then to N atoms, and ultimately recombined with holes in the Cv-C3N5 valence band. Moreover, these interfacial bonds significantly lowered the energy barrier and shortened the transport distance for electron transfer, amplifying the built-in interfacial electric field and accelerating charge dynamics. This study provides critical insights into the rational design of heterojunction photocatalysts for efficient water splitting.

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Facile synthesis of medium-entropy metal sulfides as high-efficiency cocatalysts toward photocatalytic hydrogen production Yunzhu Zang, Jiali Ren, Shanna An, Jian Tian 2025, 78:  242-251.  DOI: 10.1016/S1872-2067(25)64823-6 Abstract ( 60 )   HTML ( 2 )   PDF (2530KB) ( 15 )   Supporting Information Facing the dual challenges of environmental pollution and energy crisis, photocatalytic water splitting for hydrogen (H2) production has emerged as a promising strategy to convert solar energy into storable chemical energy. In this work, the medium-entropy metal sulfides ((FeCoNi)S2) as cocatalysts are successfully anchored onto protonated g-C3N4 nanosheets (HCN NSs) to fabricated (FeCoNi)S2-HCN composite via a solvothermal method. The photocatalytic hydrogen production rate of (FeCoNi)S2-HCN composite reaches 2996 μmol·h-1·g-1, representing 83.22, 9.16, and 1.34-fold enhancements compared to HCN (36 μmol·h-1·g-1), FeS2-HCN (327 μmol·h-1·g-1) and (FeCo)S2-HCN (2240 μmol·h-1·g-1). The apparent quantum efficiency of (FeCoNi)S2-HCN composite attains 12.29% at λ = 370 nm. Comprehensive characterizations and experimental analyses reveal that the superior photocatalytic performance stems from three synergistic mechanisms: (1) The curled-edge lamellar morphology of HCN nanosheets provides a large specific surface area, which enhances light absorption, facilitates electron transfer, and promotes cocatalyst loading. (2) (FeCoNi)S2 as cocatalyst expands the light absorption range and capacity, accelerates the separation and transfer of electron-hole pairs, and creates abundant active sites to trap photogenerated carriers for surface hydrogen evolution reactions. (3) The synergistic interactions among multiple metallic elements (Fe, Co and Ni) further enhance surface activity, increase photogenerated carrier density, and reduce charge transport resistance, ultimately optimizing hydrogen production efficiency.

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The synergistic effect of non-compensated Cu/N co-doping and graphene enhances the dual-channel generation of H2O2 over TiO2 photocatalysts Qianqian Shen, Chenlong Dong, Shilong Feng, Xueli Zhang, Qiurong Li, Jinbo Xue 2025, 78:  252-264.  DOI: 10.1016/S1872-2067(25)64799-1 Abstract ( 45 )   HTML ( 1 )   PDF (3065KB) ( 22 )   Supporting Information Modulating the electronic structure of a photocatalyst and constructing spatially separated redox sites are key strategies for achieving the photocatalytic dual-channel generation of H2O2. In this study, a graphene-modified non-compensated Cu/N-co-doped titanium dioxide (Cu-N-TiO2/rGO) photocatalyst was designed for the efficient synthesis of H2O2 via a dual-channel pathway. Precise modulation of the TiO2 conduction band position was achieved through the synergistic coupling of Cu 3d orbitals hybridized with Ti 3d orbitals and hybridization of N 2p orbitals with O 2p orbitals. This approach significantly improved the utilization of sunlight while satisfying the redox potential requirements. Cu doping not only promoted the formation of oxygen vacancies but also reduced the formation of Ti3+ ions, the photogenerated charge recombination centers. The non-compensated doping of N effectively increased the solubility of Cu2+ ions in the titanium dioxide lattice, enhanced the adsorption of hydroxyl radical intermediates, and created conditions for the subsequent hydroxyl radical combinations promoting the generation of H2O2. In addition, the introduction of highly conductive graphene improved the interfacial carrier separation efficiency while realizing the spatial separation of redox sites, creating conditions for dual-channel reactions. The experimental results showed that the H2O2 yield of Cu-N-TiO2/rGO under simulated sunlight reached 1266.7 µmol/L, which was 25.2 times higher than that of pristine TiO2. This study elucidated the synergistic mechanism of the energy band structure modulation and interfacial optimization, which provided a new idea for the design of dual-channel H2O2 production photocatalysts.

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Construction of ultrathin BiVO4 nanosheets with bismuth-oxygen dual vacancies for photocatalytic nitrogen reduction Jiahui Chen, Yue Meng, Bo Xie, Zheming Ni, Shengjie Xia 2025, 78:  265-278.  DOI: 10.1016/S1872-2067(25)64808-X Abstract ( 57 )   HTML ( 1 )   PDF (4158KB) ( 19 )   Supporting Information The efficient utilization of photogenerated electrons and the effective activation of reactive molecules are among the major challenges in photocatalytic nitrogen reduction. Defect engineering can enhance the catalyst's ability to adsorb and activate N2 and H2O, while the ultrathin structure with maximized active crystal facets can maximize the enrichment of effective photogenerated electrons. This work employs a two-step synergistic method to fabricate ultrathin BiVO4 with oxygen vacancies and bismuth vacancies (2D-VBi+O-BVO, thickness < 20 nm) for photocatalytic nitrogen reduction. Scanning electron microscopy, transmission electron microscopy (TEM), and atomic force microscopy characterization confirm the transformation of BiVO4 from bulk material (bulk-BVO, ~1300 nm) to an ultrathin structure (~15 nm). TEM, X-ray photoelectron spectroscopy, electron paramagnetic resonance characterizations, and density functional theory (DFT) calculations verify the construction of oxygen and bismuth vacancies in the ultrathin BiVO4. Compared to bulk-BVO, the photocatalytic nitrogen fixation efficiency of 2D-VBi+O-BVO is increased by 4.7 times, with the highest activity reaching 158.73 μmol·g-1·h-1. N2-temperature programmed desorption and DFT calculations demonstrate that the oxygen and bismuth vacancies in BiVO4, respectively, promote the adsorption/activation of N2 and H2O, which is crucial for the overall nitrogen reduction reaction. Photo-deposition experiments prove that the (040) plane is the active surface for electrons. And the ultrathin structure maximizes the (040) facet of BiVO4, which is conducive to the high enrichment of electrons. Meanwhile, more active sites can be exposed for the activation of N2 and H2O. In situ infrared spectroscopy confirms that N2 can be effectively adsorbed onto 2D-VBi+O-BVO, and the presence of NH2-NH2 active species is consistent with the alternating reaction pathway. This study provides new insights into the development of green and efficient photocatalysts with dual vacancies and ultrathin structures.

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Precursor and dual-template assisted synthesis of highly acidic SAPO-17 molecular sieve: Excellent NH3-SCR activity of Cu-exchanged forms Ye Wang, Pan Gao, Dan Zhao, Tongrui Liu, Sitong Zhou, Miao Yang, Shiping Liu, Bing Li, Yida Zhou, Wenhao Cui, Guangjin Hou, Peng Tian, Zhongmin Liu 2025, 78:  279-291.  DOI: 10.1016/S1872-2067(25)64801-7 Abstract ( 27 )   HTML ( 3 )   PDF (2986KB) ( 14 )   Supporting Information Silicoaluminophosphate (SAPO) molecular sieves possess diverse architectures and exceptional high-temperature hydrothermal stability, rendering them important acid catalysts. However, enhancing acid concentration of certain SAPO materials remains challenging, which limits their catalytic applications. Here, we report the synthesis of a series of SAPO materials using a developed SAPO precursor plus dual template (SPDT) strategy. A variety of SAPO materials characterized by high silica content and enhanced acidity, such as SAPO-34/56 intergrowths, SAPO-56, and SAPO-17, have been synthesized and thoroughly characterized using various techniques including integrated differential phase-contrast scanning transmission electron microscopy, two-dimensional solid-state nuclear magnetic resonance spectroscopy, and continuous rotation electron diffraction. The use of silica-enriched SAPO precursor combined with the flexible selection of the second template enables the crystalline phase regulation and improves the Si atoms incorporation into the framework. Notably, the synthesized SAPO-17 with abundant Si(4Al) species and unprecedentedly high acid density exhibits exceptional DeNOx activity after Cu loading, with NOx conversion exceeding 90% at 175-700 °C. This outstanding performance can be attributed to the unique ERI structure and the increased acidity of SAPO-17. This work not only presents an effective method for synthesizing SAPO molecular sieves with enhanced acidity but also offers a new perspective for expanding the active temperature range of the ammonia selective catalytic reduction reaction.

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Enriching framework Al sites in 8-membered rings of Cu-SSZ-39 zeolite to enhance low-temperature ammonia selective catalytic reduction performance Keyan Jin, Jinfeng Han, Yingzhen Wei, Yunzheng Wang, Jing Li, Zhongqi Liu, Yulong Shan, Ran Jia, Wenfu Yan, Jihong Yu 2025, 78:  292-302.  DOI: 10.1016/S1872-2067(25)64800-5 Abstract ( 42 )   HTML ( 2 )   PDF (2157KB) ( 14 )   Supporting Information The distributions of framework aluminum (Al) in zeolites critically govern the location and speciation of active copper (Cu) centers, thereby influencing their performance in ammonia selective catalytic reduction (NH3-SCR) of nitrogen oxides (NOₓ). Conventional Cu-SSZ-39 (Cu-SSZ-39-T) exhibits excellent hydrothermal stability but limited low-temperature activity (150-225 °C) due to a low concentration of Al in 8-membered rings (8MRs) that inhibits the formation of active [Cu(OH)]+-Z species. Herein, an SSZ-39 zeolite synthesized with potassium ions (SSZ-39-K) achieved a significantly higher 8MR Al fraction (37.6%). Density functional theory calculations and H2-temperature-programmed reduction analyses confirmed that the increased 8MR Al population facilitated the formation of [Cu(OH)]+-Z species. Aged Cu-SSZ-39-K exhibited nearly twice the NOx conversion of aged Cu-SSZ-39-T in the 150-225 °C range while maintaining comparable high-temperature activity (250-550 °C) under a gas hourly space velocity of 250,000 h-1. Enhanced low-temperature performance is particularly beneficial for mitigating NOx emissions during cold-start phase. Moreover, SSZ-39-K was synthesized with a high crystallization yield (~65%), nearly double the highest yield (33%) reported for direct synthesis routes. This work establishes a robust strategy for tailoring Al distributions in SSZ-39 zeolites, offering an effective pathway to improve low-temperature NH3-SCR performance and promote practical implementation.

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Decoupling the HOR enhancement on PtRu: Dynamically matching interfacial water to reaction coordinates Jin Liu, Zhuoyang Xie, Qiong Xiang, Xia Chen, Mengting Li, Jiawei Liu, Li Li, Zidong Wei 2025, 78:  303-312.  DOI: 10.1016/S1872-2067(25)64785-1 Abstract ( 36 )   HTML ( 1 )   PDF (1975KB) ( 7 )   Supporting Information Platinum-ruthenium alloys (PtRu) represent state-of-the-art alkaline hydrogen oxidation reaction (HOR) catalysts, yet the atomic-scale origin of their superiority over pure Pt remains incompletely understood. Here, we employ density functional theory calculations, ab initio molecular dynamics simulations, and microkinetic modeling on Pt(111) and PtRu(111) surfaces to systematically investigate the key factors, including active sites distribution, species adsorption, and solvent reorganization, that affect the HOR activity and decouple their contributions. The results reveal that while the moderate hydrogen binding energy and improved hydroxyl (OH) species adsorption both contribute to the enhanced activity, the dominant factor is the substantial reduction in solvent reorganization energy on the PtRu(111). This is facilitated by the spatial separation of active sites: Pt atoms preferentially stabilize adsorbed hydrogen, while Ru atoms strongly bind OH and interfacial water molecules. This configuration increases the probability of hydrogen interacting with OH/water and enhances the fraction of "H-up" water molecules, forming a well-organized hydrogen bond network within the electric double layer. The dynamically compatible interfacial water structure and HOR coordination promote H desorption and proton transfer in the Volmer step, thereby accelerating the HOR kinetics.

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Boosting the electrocatalytic performance of double perovskite air electrodes via Rb-doping for oxygen reduction and hydrogen production in reversible protonic ceramic electrochemical cells Chuqian Jian, Yixuan Huang, Hui Gao, Jiaojiao Xia, Wenjie Gong, Xirui Zhang, Xiaofeng Chen, Jiang Liu, Ying Liu, Yu Chen 2025, 78:  313-323.  DOI: 10.1016/S1872-2067(25)64786-3 Abstract ( 19 )   HTML ( 2 )   PDF (2967KB) ( 6 )   Supporting Information The slow oxygen reaction kinetics of air electrodes impair the performance of reversible protonic ceramic electrochemical cells (R-PCECs); hence, it is imperative to design novel air electrodes featuring excellent catalytic activity and endurance. Here, we report an Rb-doped double perovskite PrBa0.8Ca0.1Rb0.1Co2O5+δ (denoted as PBCR0.1C) as an air electrode for R-PCECs, displaying a low polarization resistance of 0.044 Ω cm2 at 700 °C and excellent stability during exposure to humid air (3 vol% H2O). The high performance is attributed to the high electrical conductivity, high concentration of oxygen vacancies, and fast surface exchange, as verified by the analyses of X-ray photoelectron spectroscopy, thermogravimetric testing, and conductivity tests. The R-PCECs with the PBCR0.1C air electrode demonstrate an encouraging performance at 700 °C: a peak power density of 2.32 W cm-2 in a fuel cell (FC) mode and an electrolysis current density of -3.55 A cm-2 at 1.3 V in an electrolysis (EL) mode. At 30 vol% steam concentration, a Faraday efficiency of 87.80% and a corresponding H2 production rate of 3.05 mL min-1 cm-2 at a current density of -0.5 A cm-2 at 650 °C. Additionally, the durability of the cell in the FC mode (120 h), EL mode (120 h), and cycling FC/EL mode (100 h) at 650 °C suggests the great potential of PBCR0.1C as the highly reactive and robust air electrodes of R-PCECs.

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Ultrafine L10 PtFeZn intermetallics via a two-step annealing process for oxygen reduction reaction: Decoupling alloying and ordering stages Yun-Fei Xia, Bo Liu, Zi-Yu Zhang, Zi-Gang Zhao, Pan Guo, Si Lin, Bing Liu, Yan Wang, Yun-Long Zhang, Lei Zhao, Li-Guang Wang, Zhen-Bo Wang 2025, 78:  324-335.  DOI: 10.1016/S1872-2067(25)64805-4 Abstract ( 55 )   HTML ( 2 )   PDF (2850KB) ( 8 )   Supporting Information In this paper, we report the design of ultrafine ordered PtFeZn ternary intermetallics uniformly supported on ZIF-8-derived Zn,N-codoped graphitic carbon (ZnNC) via a green aqueous impregnation method followed by a two-step annealing protocol (H2/Ar, 600 and 800 ℃) to circumvent the sintering issues imposed by conventional thermodynamics. Physical characterizations (X-ray diffraction, high-angle annular dark-field scanning transmission electron microscopy, X-ray absorption spectroscopy) and theoretical calculations reveal that low-temperature annealing at 600 ℃ stabilizes sub-nano disordered PtFe alloys via the strong metal-support interactions (SMSI) between Zn in ZnNC and Pt precursors, while high-temperature treatment at 800 ℃ promotes Zn diffusion from the support into the alloy bulk and simultaneously triggers the disorder-to-order phase transition. The as-prepared ZnNC-15PtFeZn exhibits an initial mass activity of 0.769 mA/μgPt and retains 61.7% of its activity after 30000 cycles of accelerated stress testing (AST). Notably, when used as a cathode catalyst in MEA, ZnNC-15PtFeZn achieves superior power density (2.018 W/cm2 under H2-O2) at half the Pt loading (0.05 mg/cm2) of state-of-the-art commercial Pt/C, highlighting its potential for low-Pt PEMFCs. Density functional theory confirms that Fe enhances ORR activity via ligand effects, while Zn strengthens Pt-Fe/Zn bonding (elevating vacancy formation energies), thereby improving structural stability. This mild, scalable aqueous impregnation strategy offers a general approach for synthesizing multi-component ordered alloys in electrocatalysis.

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Breaking the selectivity barrier in glycerol electrooxidation to glyceraldehyde via redox mediation Zhenghao Mao, Wenjing Xu, Na Han, Yanguang Li 2025, 78:  336-342.  DOI: 10.1016/S1872-2067(25)64816-9 Abstract ( 28 )   HTML ( 1 )   PDF (1544KB) ( 5 )   Supporting Information Aldehydes are valuable intermediates with widespread industrial applications, and their traditional synthesis relies on chemical oxidation that is often hazardous and environmentally unfriendly. Electrochemical oxidation offers a more sustainable and milder alternative; however, it faces challenges such as aldehyde overoxidation and susceptibility to base-catalyzed Cannizzaro disproportionation. Electrochemical glycerol oxidation to glyceraldehyde is a representative example, which typically requires precious metal-based electrocatalysts but still suffers from low selectivity and activity. Here, we report a metal-free oxidation strategy mediated by 2,2,6,6-tetramethylpiperidine-1-oxyl. By systematically investigating the redox thermodynamics and kinetics of TEMPO across a broad pH range, we construct a Pourbaix diagram and elucidate the relative kinetics of each reaction step. These insights allow us to explain the anomalously high apparent Faradaic efficiency (~200%) observed under acidic conditions, and identify neutral media as the optimal environment for selective glyceraldehyde production. Under optimized conditions, our system achieves a glyceraldehyde Faradaic efficiency exceeding 93% and a partial current density of 23.3 mA cm-2 at 0.57 V — more than doubling the performance of the best reported precious metal-based systems. Furthermore, the versatility of this strategy extends to the selective oxidation of other primary alcohols to their corresponding aldehydes with near-unity selectivity.

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Proximity-engineered Ru single-atom sites modulate Fe-N4 spatial distortion for enhanced acidic oxygen reduction reaction Shu-Hu Yin, Xiao-Yang Cheng, Yu Han, Ting Zhu, Zhong-Wei Yu, Rui Huang, Jun Xu, Yan-Xia Jiang, Shi-Gang Sun 2025, 78:  343-353.  DOI: 10.1016/S1872-2067(25)64813-3 Abstract ( 40 )   HTML ( 2 )   PDF (2249KB) ( 13 )   Supporting Information Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe-N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential (E1/2) of 0.840 V and peak power density (Pmax) of 938 mW cm-2 under 150 kPa absolute H2-O2. These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E1/2 and +42% in Pmax). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site-1 s-1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1-2 orders of magnitude (< 1 e site-1 s-1); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.