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Chinese Journal of Catalysis
2020, Vol. 41, No. 4
Online: 18 April 2020

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Cover: Zhang and coauthors in their article on pages 592-597 reported a series of Sr doped LaCo_0.8Fe_0.2O_3-δ perovskite with porous structure via a facile molten salt method,displaying higher OER activities.The authors employed high-resolution transmission electron microscopy and hard X-ray and soft X-ray absorption spectroscopy to clarify the reaction mechanism.

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Table of Contents for VOL.41 No.4 2020, 41 (4):  0-0.  Abstract ( 25 )   PDF (3197KB) ( 62 )

Special Column for the Youth Innovation Promotion Association, Chinese Academy of Sciences

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Preface to Special Column for the Youth Innovation Promotion Association, Chinese Academy of Sciences Qingde Zhang, Hongzhang Zhang 2020, 41 (4):  533-533.  DOI: 10.1016/S1872-2067(20)63553-7 Abstract ( 55 )   [Full Text(HTML)] () PDF (336KB) ( 198 )

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Piezopotential augmented photo- and photoelectro-catalysis with a built-in electric field Zhirong Liu, Xin Yu, Linlin Li 2020, 41 (4):  534-549.  DOI: 10.1016/S1872-2067(19)63431-5 Abstract ( 262 )   [Full Text(HTML)] () PDF (3750KB) ( 686 )   Rapid technological development and population growth are responsible for a series of imminent environmental problems and an ineluctable energy crisis. The application of semiconductor nanomaterials in photocatalysis or photoelectrocatalysis (PEC) for either the degradation of contaminants in the environment or the generation of hydrogen as clean fuel is an effective approach to alleviate these problems. However, the efficiency of such processes remains suboptimal for real applications. Reasonable construction of a built-in electric field is considered to efficiently enhance carrier separation and reduce carrier recombination to improve catalytic performance. In the past decade, as a new method to enhance the built-in electric field, the piezoelectric effect from piezoelectric materials has been extensively studied. In this review, we provide an overview of the properties of piezoelectric materials and the mechanisms of piezoelectricity and ferroelectricity for a built-in electric field. Then, piezoelectric and ferroelectric polarization regulated built-in electric fields that mediate catalysis are discussed. Furthermore, the applications of piezoelectric semiconductor materials are also highlighted, including degradation of pollutants, bacteria disinfection, water splitting for H2 generation, and organic synthesis. We conclude by discussing the challenges in the field and the exciting opportunities to further improve piezo-catalytic efficiency.

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Recent advance on VOCs oxidation over layered double hydroxides derived mixed metal oxides Shuangde Li, Dongdong Wang, Xiaofeng Wu, Yunfa Chen 2020, 41 (4):  550-560.  DOI: 10.1016/S1872-2067(19)63446-7 Abstract ( 141 )   [Full Text(HTML)] () PDF (1238KB) ( 427 )   Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds (VOCs) purification. Mixed metal oxides (MMOs), after topological transformation using layered double hydroxides (LDHs) as precursors, are extensively used as catalysts for VOCs oxidation due to their uniformity advantage. This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years. Particularly, it addresses the VOCs abatement performance over MMO, noble metal/MMO, core-shell structured MMO, and integral MMO film catalysts originating from LDHs. Moreover, it highlights the water vapor effect and oxidation mechanism. This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.

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Direct conversion of syngas to aromatics: A review of recent studies Xiaoli Yang, Xiong Su, De Chen, Tao Zhang, Yanqiang Huang 2020, 41 (4):  561-573.  DOI: 10.1016/S1872-2067(19)63346-2 Abstract ( 250 )   [Full Text(HTML)] () PDF (1089KB) ( 604 )   The direct catalytic conversion of syngas to aromatics offers a promising route to manufacture fine chemicals by employing non-petroleum carbon resources, because aromatic constituents are the key platform for producing polymers. However, this remains a great challenge due to the low yield of aromatics and poor catalyst stability, which restrict further development. In recent years, extensive research has been reported on the design of effective catalysts and the optimization of operating conditions to obtain better catalytic performance. In this review, we focus on these related achievements and present a comprehensive overview of different kinds of catalysts, mainly including modified Fischer-Tropsch (FT) catalysts and composite catalysts, as well as their performance and reaction mechanisms. The thermodynamic analysis of the reactions involved in this innovative conversion process and the comparison of different methods are also described in detail in this updated review. Finally, the challenges and prospects for direct syngas conversion are discussed to provide general guidelines for the construction of a well-designed reaction route.

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Layered transition-metal hydroxides for alkaline hydrogen evolution reaction Qianfeng Liu, Erdong Wang, Gongquan Sun 2020, 41 (4):  574-591.  DOI: 10.1016/S1872-2067(19)63458-3 Abstract ( 200 )   [Full Text(HTML)] () PDF (1395KB) ( 490 )   Hydrogen is a promising sustainable energy to replace fossil fuels owning to its high specific energy and environmental friendliness. Alkaline water electrolysis has been considered as one of the most prospective technologies for large scale hydrogen production. To boost the sluggish kinetics of hydrogen evolution reaction (HER) in alkaline media, abundant materials have been designed and fabricated. Herein, we summarize the key achievements in the development of layered transition-metal hydroxides[TM(OH)x] for efficient alkaline HER. Based on the structure of TM(OH)x, the mechanism of synergistic effect between TM(OH)x and HER active materials is illuminated firstly. Then, recent progress of TM(OH)x-based HER catalysts to optimize the synergistic effect are categorized as TM(OH)x and active materials, including species, structure, morphology and interaction relationship. Furthermore, TM(OH)x-based overall water splitting electrocatalysts and electrodes are summarized in the design principles for high activity and stability. Finally, some of key challenges for further developments and applications of hydrogen production are proposed.

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Understanding the origin of high oxygen evolution reaction activity in the high Sr-doped perovskite Sanzhao Song, Jing Zhou, Jian Sun, Shiyu Zhang, Xiao Lin, Zhiwei Hu, Jun Hu, Linjuan Zhang, Jian-Qiang Wang 2020, 41 (4):  592-597.  DOI: 10.1016/S1872-2067(19)63441-8 Abstract ( 166 )   [Full Text(HTML)] () PDF (1765KB) ( 369 )   Supporting Information Effective electrocatalysis is crucial for enhancing the efficiency of water splitting to obtain clean fuels. Herein, we report a system of interesting and high-performance Sr-doped perovskite electrocatalysts with porous structures, obtained via a facile molten salt method and applied in the oxygen evolution reaction (OER). With increasing the Sr content, the valence states of Co and Fe ions do not clearly increase, according to the Co-L2,3 and Fe-L2,3 as well as the Co-K and the Fe-K X-ray absorption spectroscopy, whereas doped holes are clearly observed in the O-K edge. High-resolution transmission electron microscopy indicates the appearance of an amorphous layer after the electrochemical reaction. We conclude that the formation of the amorphous layer at the surface, induced by Sr doping, is crucial for achieving high OER activity, and we offer insights into the self-reconstruction of the OER catalyst.

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Unexpectedly selective hydrogenation of phenylacetylene to styrene on titania supported platinum photocatalyst under 385 nm monochromatic light irradiation Juhong Lian, Yuchao Chai, Yu Qi, Xiangyang Guo, Naijia Guan, Landong Li, Fuxiang Zhang 2020, 41 (4):  598-603.  DOI: 10.1016/S1872-2067(19)63453-4 Abstract ( 145 )   [Full Text(HTML)] () PDF (1150KB) ( 1439 )   Supporting Information Conversion of alkynes to alkenes by photocatalysis has inspired extensive interest, but it is still challenging to obtain both high conversion and selectivity. Here we first demonstrate the photocatalytic conversion of phenylacetylene (PLE) to styrene (STE) with both high conversion and selectivity by using the titania (TiO2) supported platinum (Pt) as photocatalyst under 385 nm monochromatic light irradiation. It is demonstrated that the conversion rate of PLE is strongly dependent on the content of Pt cocatalyst loaded on the surface of TiO2. Based on our optimization, the conversion of PLE and the selectivity towards STE on the 1 wt% Pt/TiO2 photocatalyst can unexpectedly reach as high as 92.4% and 91.3%, respectively. The highly selective photocatalytic hydrogenation can well be extended to the conversion of other typical alkynes to alkenes, demonstrating the generality of selective hydrogenation of C≡C over the Pt/TiO2 photocatalyst.

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A facile solvent-free synthesis strategy for Co-imbedded zeolite-based Fischer-Tropsch catalysts for direct gasoline production Mudassar Javed, Shilin Cheng, Guihua Zhang, Cederick Cyril Amoo, Jingyan Wang, Peng Lu, Chengxue Lu, Chuang Xing, Jian Sun, Noritatsu Tsubaki 2020, 41 (4):  604-612.  DOI: 10.1016/S1872-2067(19)63436-4 Abstract ( 160 )   [Full Text(HTML)] () PDF (1146KB) ( 341 )   A series of Co-imbedded zeolite-based catalysts were synthesized following a facile solvent-free grinding route. The catalytic performance for direct syngas conversion to gasoline range hydrocarbons was compared with their counterpart Co-impregnated zeolite-based catalysts. Successful transformation of solid raw materials to targeted zeolite was confirmed by XRD, SEM, STEM, and N2 physisorption analysis. An in-depth study of acidic strength and acidic site distribution was conducted by NH3-TPD and Py-IR spectroscopy. Acidic strength showed a pivotal role in defining product range. Co@S1, with the weakest acidic strength of silicalite-1 among three types of zeolites, evaded over-cracking of product and exhibited the highest gasoline and isoparaffin selectivity (≈70% and 30.7%, respectively). Moreover, the solvent-free raw material grinding route for zeolite synthesis accompanies several advantages like the elimination of production of wastewater, high product yield within confined crystallization space, and elimination of safety concerns regarding high pressure due to the absence of the solvent. Facileness and easiness of the solvent-free synthesis route together with promising catalytic performance strongly support its application on the industrial scale.

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Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)x supported subnanometer platinum group metal catalysts Hongling Guan, Yang Chen, Chongyan Ruan, Jian Lin, Yang Su, Xiaodong Wang, Lingbo Qu 2020, 41 (4):  613-621.  DOI: 10.1016/S1872-2067(19)63489-3 Abstract ( 97 )   [Full Text(HTML)] () PDF (985KB) ( 265 )   The efficient and stable abatement of CO pollutant under ambient conditions is of great significance; however, it remains a formidable challenge. Herein, we report the versatile application of wet oxidation over Fe(OH)x supported subnanometer Pt group metal (PGM) catalysts for the complete removal of CO under ambient temperature and humidity conditions. Typically, the 1.8 wt% Rh/Fe(OH)x catalyst exhibited better durability during a~1400 min run for wet oxidation than for dry CO oxidation. Multiple characterization results including HR-TEM, H2-TPR, and in-situ DRIFTS suggested that Fe(OH)x, with good reducibility, promoted by the subnanometer Rh clusters, provided sites for the adsorption and reaction of O2 and H2O to form OH species. Subsequently, these OH species reacted with the adsorbed CO on Rh sites with a considerably lower activation energy (9 kJ mol-1) than that of dissociated O species (22 kJ mol-1), thus rationalizing the outstanding performance of Rh/Fe(OH)x for wet oxidation. Extended experiments with other PGMs revealed a good generality for the application of wet oxidation in the efficient abatement of CO under humid conditions with Fe(OH)x as the support.

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Melting-assisted solvent-free synthesis of SAPO-11 for improving the hydroisomerization performance of n-dodecane Gan Yu, Xinqing Chen, Wenjie Xue, Lixia Ge, Ting Wang, Minghuang Qiu, Wei Wei, Peng Gao, Yuhan Sun 2020, 41 (4):  622-630.  DOI: 10.1016/S1872-2067(19)63466-2 Abstract ( 102 )   [Full Text(HTML)] () PDF (1198KB) ( 315 )   A novel melting-assisted solvent-free route using solid oxalic acid was proposed for the post-treatment of SAPO-11 zeolite, followed by loading with 0.5 wt% Pt by the incipient wetness impregnation method. Subsequently, the performance of the obtained bifunctional catalysts toward the hydroisomerization of n-dodecane was examined. The prepared samples were characterized by XRD, SEM, BET, XRF, Py-IR, and solid-state NMR. From the results, it was found that the high crystallinity and uniform morphology were retained after the post-treatment and that more (002) crystal faces were exposed, which was beneficial since more acid sites were provided. More importantly, the total Brönsted acid sites and the ratio (Ra) of the micropore area to the total surface area were optimized by this method. Thus, the catalytic performance was enhanced significantly, and the prepared Pt-SAPO-11-10% catalyst had the highest i-dodecane yield of 80.1% compared to 55.3% of Pt-SAPO-11. Expectedly, this facile and cost-effective method is promising for the hydroisomerization of normal paraffin in the production of lubricant base oils.

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Effective synthesis of 5-amino-1-pentanol by reductive amination of biomass-derived 2-hydroxytetrahydropyran over supported Ni catalysts Xuemei Li, Junying Tian, Hailong Liu, Congkui Tang, Chungu Xia, Jing Chen, Zhiwei Huang 2020, 41 (4):  631-641.  DOI: 10.1016/S1872-2067(19)63471-6 Abstract ( 86 )   [Full Text(HTML)] () PDF (1529KB) ( 308 )   Supporting Information A highly efficient and green process was developed for the synthesis of useful 5-amino-1-pentanol (5-AP) from biomass-derived dihydropyran by coupling the in situ generation of 5-hydroxypentanal (5-HP, via the ring-opening tautomerization of 2-hydroxytetrahydropyran (2-HTHP)) and its reductive amination over supported Ni catalysts. The catalytic performances of the supported Ni catalysts on different oxides including SiO2, TiO2, ZrO2, γ-Al2O3, and MgO as well as several commercial hydrogenation catalysts were investigated. The Ni/ZrO2 catalyst presented the highest 5-AP yield. The characterization results of the oxide-supported Ni catalysts showed that the Ni/ZrO2 catalyst possessed high reducibility and a high surface acid density, which lead to the enhanced activity and selectivity of the catalyst. The effect of reaction parameters on the catalytic performance of the Ni/ZrO2 catalyst was studied, and a high 5-AP yield of 90.8% was achieved in the reductive amination of 2-HTHP aqueous solution under mild conditions of 80℃ and 2 MPa H2. The stability of the Ni/ZrO2 catalyst was studied using a continuous flow reactor, and only a slight decrease in the 5-AP yield was observed after a 90-h time-on-stream. Additionally, the reaction pathways for the reductive amination of 2-HTHP to synthesize 5-AP were proposed.

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The roles and mechanism of cocatalysts in photocatalytic water splitting to produce hydrogen Nan Xiao, Songsong Li, Xuli Li, Lei Ge, Yangqin Gao, Ning Li 2020, 41 (4):  642-671.  DOI: 10.1016/S1872-2067(19)63469-8 Abstract ( 411 )   [Full Text(HTML)] () PDF (2147KB) ( 953 )   Photocatalytic hydrogen (H2) evolution via water spilling over semiconductors has been considered to be one of the most promising strategies for sustainable energy supply in the future to provide non-pollution and renewable energy. The key to efficient conversion of solar-chemical energy is the design of an efficient structure for high charge separation and transportation. Therefore, cocatalysts are necessary in boosting photocatalytic H2 evolution. To date, semiconductor photocatalysts have been modified by various cocatalysts due to the extended light harvest, enhanced charge carrier separation efficiency and improved stability. This review focuses on recent developments of cocatalysts in photocatalytic H2 evolution, the roles and mechanism of the cocatalysts are discussed in detail. The cocatalysts can be divided into the following categories:metal/alloy cocatalysts, metal phosphides cocatalysts, metal oxide/hydroxide cocatalysts, carbon-based cocatalysts, dual cocatalysts, Z-scheme cocatalysts and MOFs cocatalysts. The future research and forecast for photocatalytic hydrogen generation are also suggested.

Communication

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Catalytic upgrading of ethanol to butanol over a binary catalytic system of FeNiOx and LiOH Jifeng Pang, Mingyuan Zheng, Zhinuo Wang, Shimin Liu, Xinsheng Li, Xianquan Li, Junhu Wang, Tao Zhang 2020, 41 (4):  672-678.  DOI: 10.1016/S1872-2067(20)63541-0 Abstract ( 96 )   [Full Text(HTML)] () PDF (806KB) ( 275 )   Supporting Information Catalytic conversion of ethanol to butanol is vital to bridge the gap between huge amounts of ethanol production, the limited blending ratio of ethanol in gasoline, and the outstanding performance of butanol. In this work, a highly active binary catalytic system of FeNiOx and LiOH was developed for upgrading of ethanol to butanol. After 24 h reaction at 493 K, the selectivity to butanol reached 71% with >90% high carbon alcohols at 28% ethanol conversion, which was comparable to the performance of some noble metal homogeneous catalysts.

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Insight into catalytic properties of Co3O4-CeO2 binary oxides for propane total oxidation Wenjun Zhu, Xiao Chen, Jianhui Jin, Xin Di, Changhai Liang, Zhongmin Liu 2020, 41 (4):  679-690.  DOI: 10.1016/S1872-2067(19)63523-0 Abstract ( 99 )   [Full Text(HTML)] () PDF (1282KB) ( 334 )   Supporting Information A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co) molar ratios were synthesized using a citric acid method, and their catalytic properties toward the total oxidation of propane were examined. The activities of the catalysts decrease in the order CoCeOx-70 > CoCeOx-90 > Co3O4 > CoCeOx-50 > CoCeOx-20 > CeO2. CoCeOx-70 (Co/(Ce+Co)=70% molar ratio) exhibits the highest catalytic activity toward the total oxidation of propane, of which the T90 is 310℃ (GHSV=120000 mL h-1 g-1), which is 25℃ lower than that of pure Co3O4. The enhancement of the catalytic performance of CoCeOx-70 is attributed to the strong interaction between CeO2 and Co3O4, the improvement of the low-temperature reducibility, and the increase in the number of active oxygen species. In-situ DRIFTS and reaction kinetics measurement reveal that Ce addition does not change the reaction mechanism, but promotes the adsorption and activation of propane on the catalyst surface. The addition of water vapor and CO2 in reactant gas has a negative effect on the propane conversion, and the catalyst is more sensitive to water vapor than to CO2. In addition, CoCeOx-70 exhibits excellent stability and reusability in water vapor and CO2 atmosphere.

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Rambutan-like CoP@Mo-Co-O hollow microspheres for efficient hydrogen evolution reaction in alkaline solution Wen Zhou, Mingmei Wu, Gaoren Li 2020, 41 (4):  691-697.  DOI: 10.1016/S1872-2067(20)63530-6 Abstract ( 68 )   [Full Text(HTML)] () PDF (1352KB) ( 351 )   Supporting Information Water electrolysis has attracted a lot of attention in recent years for hydrogen production. CoP has been widely investigated as a traditional electrocatalyst for hydrogen evolution reaction (HER). However, the strong bond strength of P-H bond and weak chemical stability are still the key problems in affecting catalytic performance of CoP. In this work, we synthesized rambutan-like CoP@Mo-Co-O hollow microspheres as HER electrocatalyst, solving the two problems of CoP as electrocatalyst. Benefiting from the unique three-dimensional space structure and interface effect between CoP and Mo-Co-O, the synthesized CoP@Mo-Co-O shows a small overpotential of 62 mV at the current density of 10 mA cm-2 for HER, which is much lower than the corresponding overpotential of pure CoP microspheres (117 mV). Rambutan-like CoP@Mo-Co-O hollow microspheres also show robust long-term stability and excellent cycling stability. This work provides a new method for the design and improvement of non-precious HER electrocatalysts.

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Fabrication of a solid superacid with temperature-regulated silica-isolated biochar nanosheets Zengtian Chen, Yuxue Xiao, Chao Zhang, Zaihui Fu, Ting Huang, Qingfeng Li, Yuanxiong Yao, Shutao Xu, Xiaoli Pan, Wenhao Luo, Changzhi Li 2020, 41 (4):  698-709.  DOI: 10.1016/S1872-2067(19)63522-9 Abstract ( 78 )   [Full Text(HTML)] () PDF (1889KB) ( 251 )   Supporting Information This paper reports a new strategy for the structural reconstruction of biomass carbon sulfonic acid (BCSA) to its solid superacid counterpart. In this approach, a cheap layered biomass carbon (BC) source is chemically exfoliated by cetyltrimethyl ammonium bromide and then converted to silica-isolated carbon nanosheets (CNSs) by a series of conversion steps. The state of the silica-isolated CNSs and the stacking density of their nanoparticles are regulated by the dehydration temperature. Only the highly isolated and non-crosslinked CNSs with loose particle stacking structures obtained upon dehydration at 250℃ can be turned into superacid sites (with stronger acidity than that of 100% H2SO4) after sulfonation. This is accompanied by the creation of abundant hierarchical slit pores with high external surface area, mainly driven by the strong hydrogen bonding interactions between the introduced sulfonic acid groups. In typical acid-catalyzed esterification, etherification, and hydrolysis reactions, the newly formed superacid exhibits superior catalytic activity and stability compared to those of common BCSA and commercial Amberlyst-15 catalysts, owing to its good structural stability, highly exposed stable superacidic sites, and abundance of mesoporous/macroporous channels with excellent mass transfer rate. This groundbreaking work not only provides a novel strategy for fabricating bio-based solid superacids, but also overcomes the drawbacks of BCSA, i.e., unsatisfactory structural stability, acidity, and porosity.

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SrTiO3/BiOI heterostructure: Interfacial charge separation, enhanced photocatalytic activity, and reaction mechanism Ruimin Chen, Hong Wang, Huizhong Wu, Jianping Sheng, Jieyuan Li, Wen Cui, Fan Dong 2020, 41 (4):  710-718.  DOI: 10.1016/S1872-2067(19)63472-8 Abstract ( 124 )   [Full Text(HTML)] () PDF (1858KB) ( 330 )   Supporting Information Heterostructured photocatalysts provide an effective way to achieve enhanced photocatalytic performances through efficient charge separation. Although both wide- and narrow-band-gap photocatalysts have been widely investigated, the charge separation and transfer mechanism at the contacting interface of the two has not been fully revealed. Here, a novel SrTiO3/BiOI (STB) heterostructured photocatalyst was successfully fabricated by using a facile method. The heterostructure in the photocatalyst extends the photoabsorption to the visible light range, and thus, high photocatalytic NO removal performance can be achieved under visible light irradiation. A combination of experimental and theoretical evidences indicated that the photogenerated electrons from the BiOI semiconductor can directly transfer to the SrTiO3 surface through a preformed electron delivery channel. Enhanced electron transfer was expected between the SrTiO3 and BiOI surfaces under light irradiation, and leads to efficient ROS generation and thus a high NO conversion rate. Moreover, in situ diffused reflectance infrared Fourier transform spectroscopy revealed that STB can better inhibit the accumulation of the toxic intermediate NO2 and catalyze the NO oxidation more effectively. This work presents a new insight into the mechanism of the interfacial charge separation in heterostructures and provides a simple strategy to promote the photocatalytic technology for efficient and safe air purification.

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Effect of pH on the catalytic performance of PtSn/B-ZrO2 in propane dehydrogenation Zhonghai Ji, Dengyun Miao, Lijun Gao, Xiulian Pan, Xinhe Bao 2020, 41 (4):  719-729.  DOI: 10.1016/S1872-2067(19)63395-4 Abstract ( 93 )   [Full Text(HTML)] () PDF (1170KB) ( 284 )   Boron-modified ZrO2 (B-ZrO2) was synthesized under various pH values (9, 10, and 11) and used as the supports of PtSn catalysts (PtSn/B-ZrO2-x) for non-oxidative dehydrogenation of propane. The NH3-TPD and pyridine IR show that only Lewis acid is present and the acid strength increases with the synthesis pH. PtSn/B-ZrO2-10 exhibits the best catalytic performance with an initial propane conversion of 36% and a deactivation rate constant (kd) of 0.0127 h-1. The XPS results indicate that the electronic properties of Pt and SnOx are affected not only by their interaction but also by the interaction with support. After a careful analysis of the oxygen storage capacity and activity in CO oxidation, it is hypothesized that the interaction between Pt and Sn becomes stronger following the order:PtSn/B-ZrO2-9 < PtSn/B-ZrO2-11 < PtSn/B-ZrO2-10. The characterization with TPO and Raman on spent catalysts exhibits that more hydrogen deficient coke forms on the support and less coke deposits on the metal surface of PtSn/B-ZrO2-10. The results reveal that the interaction between Pt and Sn is influenced by their respective interaction with the support and a moderate interaction between the metal species and the support is desired.