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Chinese Journal of Catalysis
2022, Vol. 43, No. 6
Online: 18 June 2022

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Cover: In this review on pages 1380–1398, Wang and co-workers discussed the recent exciting progresses of LDHs hybriding with other two-dimensional (2D) materials for overall water splitting reactions. Particularly, the structural features, morphologies, charge transfer, synergistic effects for the heterostructure/heterointerface that influence the electrocatalytic performance and the current challenges facing further application are discussed in detail.

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Editorial

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Preface to special issue on electrocatalysis for sustainable energy Bao Yu Xia, Yu Chen 2022, 43 (6):  1379-1379.  DOI: 10.1016/S1872-2067(21)64055-X Abstract ( 161 )   HTML ( 1388 )   PDF (495KB) ( 251 )

Review

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2D materials modulating layered double hydroxides for electrocatalytic water splitting Jinling Cheng, Dingsheng Wang 2022, 43 (6):  1380-1398.  DOI: 10.1016/S1872-2067(21)63987-6 Abstract ( 460 )   HTML ( 537 )   PDF (8786KB) ( 444 )   Exploring highly efficient electrochemical water splitting catalysts has recently attracted extensive research interest from both fundamental researches and practical applications. Transition metal-based layered double hydroxides (LDHs) have been proved to be one of the most efficient materials for oxygen evolution reaction (OER), however, still suffered from low conductivity and sluggish kinetics for hydrogen evolution reaction (HER), which largely inhibited the overall water splitting efficiency. To address this dilemma, enormous approaches including doping regulation, intercalation tuning and defect engineering are therefore rationally designed and developed. Herein, we focus on the recent exciting progress of LDHs hybridization with other two-dimensional (2D) materials for water splitting reactions, not barely for enhancing OER efficiency but also for boosting HER activity. Particularly, the structural features, morphologies, charge transfer and synergistic effects for the heterostructure/heterointerface that influence the electrocatalytic performance are discussed in details. The hybrid 2D building blocks not only serve as additional conductivity and structural supported but also promote electron transfer at the interfaces and further enhance the electrocatalytic performance. The construction and application of the nanohybrid materials will guide a new direction in developing multifunctional materials based on LDHs, which will contribute to energy conversion and storage.

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Electrocatalytic generation of reactive species and implications in microbial inactivation Forrest Nichols, Kenneth I. Ozoemena, Shaowei Chen 2022, 43 (6):  1399-1416.  DOI: 10.1016/S1872-2067(21)63941-4 Abstract ( 152 )   HTML ( 370 )   PDF (6520KB) ( 150 )   Controlling microbial proliferation in water systems, including wastewater, recreational water, and drinking water, is essential to societal health. Microbial inactivation through electrochemically generated reactive species (RS) mediated pathways provides an effective route toward this microbial control. Herein we provide an overview of recent progress toward electrocatalytic generation of RS and their application in water disinfection, with a focus on the selective production of RS, the microorganism interactions with RS (including both RS mechanisms of action and innate microorganism responses to RS), and practical implementation of electrochemically generated RS for microbial inactivation. The article is concluded with a perspective where the challenges and opportunities of RS-based electrochemical disinfection of water are highlighted, along with possible future research directions.

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Structural and interfacial engineering of well-defined metal-organic ensembles for electrocatalytic carbon dioxide reduction Fenglei Lyu, Wei Hua, Huirong Wu, Hao Sun, Zhao Deng, Yang Peng 2022, 43 (6):  1417-1432.  DOI: 10.1016/S1872-2067(21)63980-3 Abstract ( 397 )   HTML ( 234 )   PDF (23960KB) ( 348 )   Electrochemical carbon dioxide reduction (CO2RR) has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals. However, the large-scale implementation of CO2RR is severely hindered by the lack of high-performance CO2RR electrocatalysts. Heterogeneous molecular catalysts and metal-organic framework with well-defined structure and high tunability of the metal centers and ligands show great promise for CO2RR in terms of both fundamental understanding and practical application. Here, structural and interfacial engineering of these well-defined metal-organic ensembles is summarized. This review starts from the fundamental electrochemistry of CO2RR and its evaluation criteria, and then moves to the heterogeneous molecular catalysts and metal-organic framework with emphasis on the engineering of metal centers and ligands, their interaction with supports, as well as in situ reconstruction of metal-organic ensembles. Summary and outlook are present in the end, with the hope to inspire and provoke more genuine thinking on the design and fabrication of efficient CO2RR electrocatalysts.

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Oxygen reduction reaction on Pt-based electrocatalysts: Four-electron vs. two-electron pathway Lili Zhang, Suyu Jiang, Wei Ma, Zhen Zhou 2022, 43 (6):  1433-1443.  DOI: 10.1016/S1872-2067(21)63961-X Abstract ( 348 )   HTML ( 195 )   PDF (3574KB) ( 419 )   Oxygen reduction reaction (ORR) has attracted extensive attention as an important component for sustainable energy storage and conversion technologies. However, the sluggish kinetics has hampered the practical application. Pt-based nanomaterials have triggered much interest as the most promising electrocatalyst to facilitate the kinetics of ORR. Nonetheless, a major challenge for Pt-based electrocatalysts is to precisely control the selectivity of reaction pathways and possible products (H2O or H2O2) with a reduced loading amount of precious Pt. This review systematically summarizes the strategies to regulate the ORR performances of Pt-based electrocatalysts by accommodating the adsorption energy and spatial structure. Further discussion is implemented about the key factors to accelerate the kinetics of ORR and control the 4e-ORR and 2e-ORR pathways. Finally, we demonstrate the challenges and perspectives for further development of novel Pt-based electrocatalysts.

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Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction Jingsen Bai, Liting Yang, Zhao Jin, Junjie Ge, Wei Xing 2022, 43 (6):  1444-1458.  DOI: 10.1016/S1872-2067(21)63991-8 Abstract ( 268 )   HTML ( 222 )   PDF (4347KB) ( 274 )   Proton exchange membrane fuel cells (PEMFCs) are considered ideal energy-conversion devices because of their environmentally friendly nature and high theoretical energy efficiency. However, cathodic polarization, which is a result of the sluggish oxygen reduction reaction (ORR) kinetics, is a significant source of energy loss and reduces fuel cell efficiency. Further, the need to use Pt in commercial Pt/C cathodes has restricted their large-scale application in fuel cells because of its high cost and poor durability. Thus, improvements in the activity and durability of Pt-based catalyst are required to reduce the amount of Pt required and, thus, costs, while increasing the ORR rate and fuel cell power density and promoting widespread PEMFC commercialization. In recent years, atomically ordered Pt-based intermetallic nanocrystals have received tremendous attention owing to their excellent activity and stability for the ORR. Therefore, in this review, we first introduce the formation of intermetallic compounds from the perspective of thermodynamics and kinetics to lay a theoretical foundation for the design of these compounds. In addition, optimization strategies for Pt-based ordered intermetallic catalysts are summarized in terms of the catalyst composition, size, and morphology. Finally, we conclude with a discussion of the current challenges and future prospects of Pt-based ordered alloys. This review is designed to help readers gain insights into the recent developments in and rational design of Pt-based intermetallic nanocrystals for the ORR and encourage research that will enable the commercialization of PEMFCs.

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Rational design and synthesis of one-dimensional platinum-based nanostructures for oxygen-reduction electrocatalysis Huiting Niu, Chenfeng Xia, Lei Huang, Shahid Zaman, Thandavarayan Maiyalagan, Wei Guo, Bo You, Bao Yu Xia 2022, 43 (6):  1459-1472.  DOI: 10.1016/S1872-2067(21)63862-7 Abstract ( 277 )   HTML ( 229 )   PDF (5357KB) ( 430 )   Fuel cells have attracted extensive attention due to their high conversion efficiency and environmental friendliness. However, their wider application is limited by the poor activity and high cost of platinum (Pt), which is widely used as the cathode catalyst to overcome the slow kinetics associated with oxygen reduction reaction (ORR). Pt-based composites with one-dimensional (1D) nanoarchitectures demonstrate great advantages towards efficient ORR catalysis. This review focuses on the recent advancements in the design and synthesis of 1D Pt-based ORR catalysts. After introducing the fundamental ORR mechanism and the advanced 1D architectures, their synthesis strategies (template-based and template-free methods) are discoursed. Subsequently, their morphology and structure optimization are highlighted, followed by the superstructure assembly using 1D Pt-based blocks. Finally, the challenges and perspectives on the synthesis innovation, structure design, physical characterization, and theoretical investigations are proposed for 1D Pt-based ORR nanocatalysts. We anticipate this study will inspire more research endeavors on efficient ORR nanocatalysts in fuel cell application.

Communication

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Probing the role of surface speciation of tin oxide and tin catalysts on CO2 electroreduction combining in situ Raman spectroscopy and reactivity investigations Ming He, Bingjun Xu, Qi Lu 2022, 43 (6):  1473-1477.  DOI: 10.1016/S1872-2067(21)64014-7 Abstract ( 397 )   HTML ( 235 )   PDF (1431KB) ( 569 )   Supporting Information Electrochemical CO2 reduction to formate is a promising approach to store renewable electricity and utilize CO2. Tin oxide catalysts are efficient catalysts for this process, while the mechanisms underneath, especially the existence and role of oxidized tin species under CO2 electroreduction conditions remain unclear. In this work, we provide strong evidence on the presence of oxidized tin species on both SnO2 and Sn during CO2 reduction via in situ surface-enhanced Raman spectroscopy, while in different nature. Reactivity measurements show similar activity and selectivity to formate production on SnO2 and Sn catalysts. Combined analysis of Raman spectra and reactivity results suggests that Sn(IV) and Sn(II) oxide species are unlikely the catalytic species in CO2 electroreduction to formate.

Article

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Copper-doped nickel oxyhydroxide for efficient electrocatalytic ethanol oxidation Huining Wang, Anxiang Guan, Junbo Zhang, Yuying Mi, Si Li, Taotao Yuan, Chao Jing, Lijuan Zhang, Linjuan Zhang, Gengfeng Zheng 2022, 43 (6):  1478-1484.  DOI: 10.1016/S1872-2067(21)63995-5 Abstract ( 392 )   HTML ( 214 )   PDF (2207KB) ( 352 )   Supporting Information Rational design of low-cost and efficient electrocatalysts for ethanol oxidation reaction (EOR) is imperative for electrocatalytic ethanol fuel cells. In this work, we developed a copper-doped nickel oxyhydroxide (Cu-doped NiOOH) catalyst via in situ electrochemical reconstruction of a NiCu alloy. The introduction of Cu dopants increases the specific surface area and more defect sites, as well as forms high-valence Ni sites. The Cu-doped NiOOH electrocatalyst exhibited an excellent EOR performance with a peak current density of 227 mA·cm -2 at 1.72 V versus reversible hydrogen electrode, high Faradic efficiencies for acetate production (> 98%), and excellent electrochemical stability. Our work suggests an attractive route of designing non-noble metal based electrocatalysts for ethanol oxidation.

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Surface chlorine doped perovskite-type cobaltate lanthanum for water oxidation Wei Shen, Jing Jin, Yang Hu, Yichao Hou, Jie Yin, Zhenhui Ma, Yong-Qing Zhao, Pinxian Xi 2022, 43 (6):  1485-1492.  DOI: 10.1016/S1872-2067(21)64004-4 Abstract ( 222 )   HTML ( 229 )   PDF (7273KB) ( 247 )   Supporting Information Rationally manipulating the in-situ formed catalytically active surface of catalysts remains a great challenge for a highly efficient water electrolysis. Here, we report a cationic oxidation method which can adjust the leaching of the in-situ catalyst and promote the reconstruction of dynamic surface for the oxygen evolution reaction (OER). The chlorine doping can reduce the possibility of triggering in-situ cobalt oxidation and chlorine leaching, leading to a transformation of the surface chlorine doped LaCoO3 (Cl-LaCoO3) into an intricate amorphous (oxygen) hydroxide phase. And thus, Cl-LaCoO3 nanocrystals shows an ultralow overpotential of 342 mV at the current density of 10 mA cm -2 and Tafel slope of 76.2 mV dec-1. Surface reconstructed Cl-LaCoO3 is better than many of the most advanced OER catalysts and has proven significant stability. This work provides a new prospect for designing a high-efficiency electrocatalyst with optimized perovskite-structure in renewable energy system.

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A trace of Pt can significantly boost RuO2 for acidic water splitting Qing Yao, Jiabo Le, Shize Yang, Jun Cheng, Qi Shao, Xiaoqing Huang 2022, 43 (6):  1493-1501.  DOI: 10.1016/S1872-2067(21)63952-9 Abstract ( 262 )   HTML ( 126 )   PDF (5318KB) ( 334 )   Supporting Information The development of highly potential electrocatalysts for acidic water electrolysis is particularly desirable for many energy-related processes. Herein, we demonstrated a versatile strategy to activate and stabilize RuO2-based electrocatalyst for acidic water splitting by a trace of Pt, where Pt plays an essential role in promoting oxygen evolution reaction (OER), and can simultaneously act as the active site for hydrogen evolution reaction (HER). Compared with pure Ru oxide nanosheet assemblies (Ru ONAs), the “5%Pt-containing” Ru ONAs (5%Pt-Ru ONAs) achieve much enhanced OER activity in 0.5 and 0.05 mol/L H2SO4, with much lower overpotentials of 227 and 234 mV at 10 mA cm‒2, respectively. Experimental and theoretical analyses reveal that the atomically dispersed Pt incorporating into RuO2 lattice is conducive to increasing the concentration of O vacancies, which effectively enhances the interaction with reaction intermediate and thus lowers the energy barrier for the formation of OOH*. Moreover, benefited from the presence of Pt, the formation of RuO2 is more achievable when proper annealing is applied. In addition to OER, due to the presence of active Pt, the HER performance of 5%Pt-Ru ONAs can also be ensured, thereby realizing efficient acidic overall water splitting. Finally, the excellent activity can also be achieved without sacrificing stability. This work highlights an attractive strategy for designing active and stable RuO2-based electrocatalysts for acidic overall water splitting.

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Atomic modulation of Fe-Co pentlandite coupled with nitrogen-doped carbon sphere for boosting oxygen catalysis Si-Jie Li, Yong Xie, Bi-Lin Lai, Yingmin Liang, Kang Xiao, Ting Ouyang, Nan Li, Zhao-Qing Liu 2022, 43 (6):  1502-1510.  DOI: 10.1016/S1872-2067(21)63932-3 Abstract ( 260 )   HTML ( 126 )   PDF (2405KB) ( 256 )   Supporting Information Reversible oxygen reaction plays a crucial role in rechargeable battery systems, but it is limited by the slow reaction kinetics. Herein, the ionic modulation of cobalt pentlandite coupled with nitrogen-doped bowl-like hollow carbon sphere is well designed on octahedral and tetrahedral sites. The robust FexCo9-xS8-NHCS-V with iron replacing at the octahedron possesses prolonged metal sulfur bond and exhibits excellent bifunctional electrocatalytic performance towards oxygen reduction reaction (ORR, E1/2 = 0.80 V vs. RHE) and excellent oxygen evolution reaction (OER, Ej = 10 = 1.53 V vs. RHE) in 0.1 mol/L KOH. Accordingly, a rechargeable Zn-air battery of FexCo9-xS8-NHCS-V cathode endows high energy efficiency (102 mW cm-2), and a microbial fuel cell achieves a high-power density (791 ± 42 mW m -2), outperforming the benchmark Pt/C catalyst.

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N-doped porous carbon nanofibers inlaid with hollow Co3O4 nanoparticles as an efficient bifunctional catalyst for rechargeable Li-O2 batteries Hongbin Chen, Yaqian Ye, Xinzhi Chen, Lili Zhang, Guoxue Liu, Suqing Wang, Liang-Xin Ding 2022, 43 (6):  1511-1519.  DOI: 10.1016/S1872-2067(21)64017-2 Abstract ( 240 )   HTML ( 126 )   PDF (4036KB) ( 245 )   Supporting Information Stable and high-efficiency bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are desired for the practical application of Li-O2 batteries with excellent rate performance and cycle stability. Herein, a novel hybrid bifunctional catalyst with carbon nanofibers inlaid with hollow Co3O4 nanoparticles and separate active sites for ORR and OER were prepared and applied in Li-O2 batteries. Benefiting from the synergistic effect of unique porous structural features and high electrocatalytic activity of hollow Co3O4 intimately bound to N-doped carbon nanofibers, the assembled Li-O2 batteries with novel catalyst exhibited high specific capacity, excellent rate capability, and cycle stability up to 150 cycles under a capacity limitation of 500 mAh g-1 at a current density of 100 mA g-1. The facile synthesis and preliminary results in this work show the as-prepared catalyst as a promising bifunctional electrocatalyst for applications in metal-air batteries, fuel cells, and electrocatalysis.

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1T′-MoTe2 monolayer: A promising two-dimensional catalyst for the electrochemical production of hydrogen peroxide Xiaoxu Sun, Xiaorong Zhu, Yu Wang, Yafei Li 2022, 43 (6):  1520-1526.  DOI: 10.1016/S1872-2067(21)64007-X Abstract ( 207 )   HTML ( 124 )   PDF (3703KB) ( 172 )   Supporting Information The direct synthesis of hydrogen peroxide (H2O2) via a two-electron oxygen reduction reaction (2e-ORR) in acidic media has emerged as a green process for the production of this valuable chemical. However, such an approach employs expensive noble-metal-based electrocatalysts, which severely undermines its feasibility when implemented on an industrial scale. Herein, based on density functional theory computations and microkinetic modeling, we demonstrate that a novel two-dimensional (2D) material, namely a 1T′-MoTe2 monolayer, can serve as an efficient non-precious electrocatalyst to facilitate the 2e-ORR. The 1T′-MoTe2 monolayer is a stable 2D crystal that can be easily produced through exfoliation techniques. The surface-exposed Te sites of the 1T′-MoTe2 monolayer exhibit a favorable OOH* binding energy of 4.24 eV, resulting in a rather high basal plane activity toward the 2e-ORR. Importantly, kinetic computations indicate that the 1T'-MoTe2 monolayer preferentially promotes the formation of H2O2 over the competing four-electron ORR step. These desirable characteristics render 1T′-MoTe2 a promising candidate for catalyzing the electrochemical reduction of O2 to H2O2.

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Manipulating the electronic structure of Ni electrocatalyst through d-p orbital hybridization induced by B-doping for efficient alkaline hydrogen oxidation reaction Pengyu Han, Na Yao, Wei Zuo, Wei Luo 2022, 43 (6):  1527-1534.  DOI: 10.1016/S1872-2067(21)63955-4 Abstract ( 357 )   HTML ( 139 )   PDF (7525KB) ( 304 )   Supporting Information Developing highly efficient platinum-group-metal-free electrocatalysts towards hydrogen oxidation reaction (HOR) under alkaline electrolyte is critical for the development of alkaline exchange member fuel cells. Herein, we reported the synthesis of boron doped Ni electrocatalyst (B-Ni/C) and its remarkable alkaline HOR performance, with a 10-fold mass activity enhancement compared with that of undoped Ni catalyst. Experimental results and density functional theory calculations indicate the d-p hybridization between the p orbital of B and the d orbital of Ni via B-doping could lead to promoted OH adsorption and optimized hydrogen binding energy on Ni surface, which together with the reduced formation energy of water species, contributes to the enhanced HOR performance under alkaline electrolyte.

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Nitrogen-doped graphene aerogel-supported ruthenium nanocrystals for pH-universal hydrogen evolution reaction Yu Ding, Kai-Wen Cao, Jia-Wei He, Fu-Min Li, Hao Huang, Pei Chen, Yu Chen 2022, 43 (6):  1535-1543.  DOI: 10.1016/S1872-2067(21)63977-3 Abstract ( 256 )   HTML ( 131 )   PDF (6730KB) ( 454 )   Supporting Information The design and synthesis of high-performance and low-cost electrocatalysts for the hydrogen evolution reaction (HER), a key half-reaction in water electrolysis, are essential. Owing to their modest hydrogen adsorption energy, ruthenium (Ru)-based nanomaterials are considered outstanding candidates to replace the expensive platinum (Pt)-based HER electrocatalysts. In this study, we developed an adsorption-pyrolysis method to construct nitrogen (N)-doped graphene aerogel (N-GA)-supported ultrafine Ru nanocrystal (Ru-NC) nanocomposites (Ru-NCs/N-GA). The particle size of the Ru-NCs and the conductivity of the N-GA substrate can be controlled by varying the pyrolysis temperature. Optimal experiments reveal revealed that 10 wt% Ru-NCs/N-GA nanocomposites require overpotentials of only 52 and 36 mV to achieve a current density of 10 mA cm-2 in 1 mol/L HClO4 and 1 mol/L KOH electrolytes for HER, respectively, which is comparable to 20 wt% Pt/C electrocatalyst. Benefiting from the ultrafine size and uniform dispersion of the Ru-NCs, the synergy between Ru and the highly conductive substrate, and the anchoring effect of the N atom, the Ru-NCs/N-GA nanocomposites exhibit excellent activity and durability in the pH-universal HER, thereby opening a new avenue for the production of commercial HER electrocatalysts.