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Chinese Journal of Catalysis
2020, Vol. 41, No. 3
Online: 18 March 2020

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Cover: Fu and coworks in their Article on pages 404-414 reported the one-pot conversion of xylose to furfuryl alcohol over bifunctional Cu/SBA-15-SO₃H catalyst.The co-existed acidic -SO₃H sites and Cu sites kept a balance and cooperatively catalyzed the cascade conversion.

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Table of Contents for VOL.41 No.3 2020, 41 (3):  0-0.  Abstract ( 27 )   PDF (3379KB) ( 94 )

Reviews

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Direct liquefaction techniques on lignite coal: A review Arif Ali, Chen Zhao 2020, 41 (3):  375-389.  DOI: 10.1016/S1872-2067(19)63492-3 Abstract ( 135 )   [Full Text(HTML)] () PDF (935KB) ( 375 )   With the pressure owing to fossil oil shortages, direct liquefaction is attracting significant attention as a highly efficient and low-cost technique for lignite-to-fuel conversion. In this review, the diverse catalytic systems and mechanisms involved in lignite liquefaction are reviewed. The top five global technologies include IGOR (Germany), HTI (the USA), FFI (Russia), NEDOL (Japan), and Shenhua (China), which have already been applied in industrial scales. Among the five technologies, Shenhua (China) outputs as high as 3000 t/d using a suspended bed reactor, iron-based catalyst, and rehydrogenated recycled solvents (paraffin, aromatics, etc.). The conversion of lignite is quite difficult due to the presence of ionic bond and non-covalent interactions, such as hydrogen bonding; thus, it is well recognized that the catalytic liquefaction under relatively mild conditions is more feasible than non-catalytic liquefaction. Iron-based catalysts can efficiently facilitate the lignite liquefaction and promote the lignite cracking aided by a hydrogen-donor solvent; thus, they have attracted interest from researchers globally. The different liquefaction mechanisms of lignite including free radical, oxidation, alkanolysis, and hydrogenation lead to the corresponding products:preasphaltene and asphaltene, mixed carboxylic acids, mixed esters and ethers, and cyclic compounds, respectively. Therefore, the catalytic system of the lignite liquefaction process would be accordingly optimized and modified to afford different products.

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Micro-nanostructural designs of bifunctional electrocatalysts for metal-air batteries Fang Shi, Xuefeng Zhu, Weishen Yang 2020, 41 (3):  390-403.  DOI: 10.1016/S1872-2067(19)63514-X Abstract ( 194 )   [Full Text(HTML)] () PDF (3488KB) ( 461 )   Water-based rechargeable metal-air batteries play an important role in the storage and conversion of renewable electric energy. However, the sluggish kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have limited the practical application of rechargeable metal-air batteries. Most of reviews were focused on single functional electrocatalysts while few on bifunctional electrocatalysts. It is indispensable but challenging to design a bifunctional electrocatalyst that is active and stable to the two reactions. Recently, attempts to develop high active bifunctional electrocatalysts for both ORR and OER increase rapidly. Much work is focused on the micro-nano design of advanced structures to improve the performance of bifunctional electrocatalyst. Transition-metal materials, carbon materials and composite materials, and the methods developed to prepare micro-nano structures, such as electrochemical methods, chemical vapor deposition, hydrothermal methods and template methods are reported in literatures. Additionally, many strategies, such as adjustments of electronic structures, oxygen defects, metal-oxygen bonds, interfacial strain, nano composites, heteroatom doping etc., have been used extensively to design bifunctional electrocatalysts. To well understand the achievements in the recent literatures, this review focuses on the micro-nano structural design of materials, and the related methods and strategies are classed into two groups for the improvement of intrinsic and apparent activities. The fine adjustment of nano structures and an in-depth understanding of the reaction mechanism are also discussed briefly.

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One-pot cascade conversion of xylose to furfuryl alcohol over a bifunctional Cu/SBA-15-SO3H catalyst Tianyu Deng, Guangyue Xu, Yao Fu 2020, 41 (3):  404-414.  DOI: 10.1016/S1872-2067(19)63505-9 Abstract ( 123 )   [Full Text(HTML)] () PDF (1370KB) ( 436 )   Supporting Information The conversion of hemicellulose-derived xylose to furfuryl alcohol is a practical procedure for producing value-added chemicals from biomass. In this study, a bifunctional Cu/SBA-15-SO3H catalyst was employed for the one-pot catalytic conversion of xylose to furfuryl alcohol with a yield of up to 62.6% at the optimized conditions of 140℃, 4 MPa, and for 6 h in a biphasic water/n-butanol solvent. A high reaction temperature resulted in further hydrogenation to 2-methyl furan, while a high hydrogen pressure led to a side hydrogenation reaction to xylitol. The biphasic solvent allowed xylose solvation as well as furfuryl product extraction. The acidic -SO3H sites and Cu sites co-existed, maintained a balance, and cooperatively catalyzed the cascade conversion. Excessive acidic sites and large pores could promote the xylose conversion, although a low furfuryl alcohol yield was obtained. This catalytic system could be potentially applied to the one-pot synthesis of furfuryl alcohol from hemicellulose-derived xylose.

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Unveiling the decomposition mechanism of formic acid on Pd/WC(0001) surface by using density function theory Jinhua Zhang, Yuanbin She 2020, 41 (3):  415-425.  DOI: 10.1016/S1872-2067(19)63463-7 Abstract ( 107 )   [Full Text(HTML)] () PDF (1987KB) ( 245 )   In pursuit of low-cost direct formic acid fuel cells, tungsten carbide (WC) supported Pd catalyst is considered as an ideal candidate for efficient decomposition of formic acid due to low Pd utilization and excellent performance. Herein, different adsorption configurations and active sites of the intermediates, involved in the HCOOH decomposition, on WC(0001)-supported Pd monolayer (Pd/WC(0001)) surface investigated by using density functional theory. The results reveal that trans-HCOOH, HCOO, cis-COOH, trans-COOH, HCO, CO, H2O, OH and H exhibit chemisorption on Pd/WC(0001) surface, whereas cis-HCOOH and CO2 exhibit weak interactions with Pd/WC(0001) surface. In addition, the minimum energy pathways of HCOOH decomposition are analyzed to generate CO and CO2 due to the fracture of C-H, H-O and C-O bonds. The adsorbed HCOOH, HCOO, mHCOO, cis-COOH and trans-COOH configurations exhibit dissociation rather than desorption. CO formation occurs through the decomposition of cis-COOH, trans-COOH and HCO, whereas the CO2 formation happens due to the decomposition of HCOO. It is found that the most favorable pathway for HCOOH decomposition on Pd/WC(0001) surface is HCOOH→HCOO→CO2, where the formation of CO2 from HCOO dehydrogenation determines the reaction rate. Overall, CO2 is the most dominant product of HCOOH decomposition on Pd/WC(0001) surface. The presence of WC, as monolayer Pd carrier, does not alter the catalytic behavior of Pd and significantly reduces the Pd utilization.

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Novel indirect Z-scheme g-C3N4/Bi2MoO6/Bi hollow microsphere heterojunctions with SPR-promoted visible absorption and highly enhanced photocatalytic performance Ning Li, Hang Gao, Xin Wang, Sujun Zhao, Da Lv, Guoqing Yang, Xueyun Gao, Haikuan Fan, Yangqin Gao, Lei Ge 2020, 41 (3):  426-434.  DOI: 10.1016/S1872-2067(19)63478-9 Abstract ( 76 )   [Full Text(HTML)] () PDF (1662KB) ( 378 )   The surface plasmonic resonance (SPR) effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate. In this study, a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi (CN/BMO/Bi) hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods. The results revealed that the optimal ternary 0.4CN/BMO/9Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B (RhB) degradation with nine times that of pure BMO. The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4CN/BMO/9Bi is a z-scheme structure. Quenching experiments also provided solid evidence that the ·O2- (at -0.33 eV) is the main species during dye degradation, and the conduction band of g-C3N4 is only the reaction site, demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2MoO6/Bi is through an indirect z-scheme structure. Thus, the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping, resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers. The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.

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Selective synthesis of Sb2S3 nanostructures with different morphologies for high performance in dye-sensitized solar cells Xue Chen, Xuemin Li, Pengkun Wei, Xiaoyong Ma, Qinlin Yu, Lu Liu 2020, 41 (3):  435-441.  DOI: 10.1016/S1872-2067(19)63493-5 Abstract ( 58 )   [Full Text(HTML)] () PDF (1240KB) ( 254 )   Supporting Information In this work, we initially synthesized Sb2S3 with uniform flower-like structures via a facile hydrothermal method through the modification of the Sb source and pH value. Afterward, Sb2S3 with a nanosheet structure was successfully synthesized on reduced graphene oxide (Sb2S3@RGO). The flower-like Sb2S3 and the Sb2S3@RGO nanosheets were tested as the counter electrode (CE) of dye-sensitized solar cells, and the latter exhibited a higher electrocatalytic property than the former owing to the introduction of graphene. The results from electrochemical tests indicated that the as-prepared Sb2S3@RGO nanosheets possess higher catalytic activity, charge-transfer ability, and electrochemical stability than Sb2S3, RGO, and Pt CEs. More notably, the power conversion efficiency of Sb2S3@RGO reached 8.17%, which was higher than that of the standard Pt CE (7.75%).

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Co-Cr-O mixed oxides for low-temperature total oxidation of propane: Structural effects, kinetics, and spectroscopic investigation Wen-Min Liao, Pei-Pei Zhao, Bing-Heng Cen, Ai-Ping Jia, Ji-Qing Lu, Meng-Fei Luo 2020, 41 (3):  442-453.  DOI: 10.1016/S1872-2067(19)63480-7 Abstract ( 90 )   [Full Text(HTML)] () PDF (1113KB) ( 342 )   Supporting Information A series of Co-Cr-O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane. The reaction behaviors are closely related to the structural features of the mixed oxides. The catalyst with a Co/Cr molar ratio of 1:2 (1Co2Cr) and a spinel structure has the best activity (with a reaction rate of 1.38 μmol g-1 s-1 at 250℃), which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility, as evidenced by the temperature-programmed desorption of ammonia, reduction of hydrogen, and surface reaction of propane. Kinetic study shows that the reaction orders of propane and oxygen on the 1Co2Cr catalyst (0.58 ± 0.03 and 0.34 ±0.05, respectively) are lower than those on the 2Co1Cr catalyst (0.77 ±0.02 and 0.98 ±0.16, respectively) and 1Co5Cr (0.66 ±0.05 and 1.30 ±0.11, respectively), indicating that the coverages of propane and oxygen on 1Co2Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility. In addition, in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1Co2Cr during the reaction are polydentate carbonate species, which accumulate on the surface at low temperatures (< 250℃) but decompose at relatively high temperatures.

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Fabrication of hierarchical ZnIn2S4@CNO nanosheets for photocatalytic hydrogen production and CO2 photoreduction Kai Zhu, Jie Ou-Yang, Qian Zeng, Sugang Meng, Wei Teng, Yanhua Song, Sheng Tang, Yanjuan Cui 2020, 41 (3):  454-463.  DOI: 10.1016/S1872-2067(19)63494-7 Abstract ( 73 )   [Full Text(HTML)] () PDF (1191KB) ( 361 )   Supporting Information Photocatalytic H2 production and CO2 reduction have attracted considerable attention for clean energy development. In this work, we designed an efficient photocatalyst by integrating lamellar oxygen-doped carbon nitride (CNO) nanosheets into ZnIn2S4 (ZIS) microflowers by a one-step hydrothermal method. A well-fitted 2D hierarchical hybrid heterostructure was fabricated. Under visible light irradiation, the ZIS@CNO composite with 40 wt% CNO (ZC 40%) showed the highest hydrogen evolution rate from water (188.4 μmol·h-1), which was approximately 2.1 times higher than those of CNO and ZIS (88.6 and 90.2 μmol·h-1, respectively). Furthermore, the selective CO production rates of ZC 40% (12.69 μmol·h-1) were 2.2 and 14.0 times higher than those of ZIS (5.85 μmol·h-1) and CNO (0.91 μmol·h-1), respectively, and the CH4 production rate of ZC 40% was 1.18 μmol·h-1. This enhanced photocatalytic activity of CNO@ZIS is due mainly to the formation of a heterostructure that can promote the transfer of photoinduced electrons and holes between CNO and ZIS, thereby efficiently avoiding recombination of electron-hole pairs.

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BiOCl-Bi12O17Cl2 nanocomposite with high visible-light photocatalytic activity prepared by an ultrasonic hydrothermal method for removing dye and pharmaceutical Zeqing Long, Guang Xian, Guangming Zhang, Tao Zhang, Xuemei Li 2020, 41 (3):  464-473.  DOI: 10.1016/S1872-2067(19)63474-1 Abstract ( 68 )   [Full Text(HTML)] () PDF (2057KB) ( 313 )   A BiOCl-Bi12O17Cl2 nanocomposite with a high visible-light response and a low photoinduced electron-hole pair recombination rate was successfully synthesized using an ultrasonic-hydrothermal method. The texture, structure, optical, and photocatalytic properties of the composite were characterized. The results showed that the composite had a sheet flower-like structure with a large specific surface area. Ultraviolet-visible diffuse reflection spectra and photoluminescence spectra showed that the composite had an excellent visible-light response and a low recombination rate of photoinduced electron hole pairs. The photocatalytic property of the composite was evaluated by the removal efficiency of rhodamine B and ciprofloxacin under visible-light illumination. The composite's reaction rate constant of removing rhodamine B (/ciprofloxacin) was approximately 8.14 (/4.94), 42.63 (/11.91) and 64.66 (/36.07) times that of Bi12O17Cl2, P25, and BiOCl, respectively. Furthermore, the composite showed a wide applicable pH range and excellent reusability. Mechanism analysis showed that photogenerated holes played a dominant role and ·O2- also contributed to photocatalytic degradation. In summary, this study presents a high-efficiency photocatalyst for wastewater treatment.

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Enhanced visible-light photocatalytic degradation and disinfection performance of oxidized nanoporous g-C3N4 via decoration with graphene oxide quantum dots Jing Xu, Jin Huang, Zhouping Wang, Yongfa Zhu 2020, 41 (3):  474-484.  DOI: 10.1016/S1872-2067(19)63501-1 Abstract ( 138 )   [Full Text(HTML)] () PDF (1343KB) ( 380 )   Supporting Information Oxidized nanoporous g-C3N4 (PCNO) decorated with graphene oxide quantum dots (ox-GQDs) was successfully prepared by a facile self-assembly method. As co-catalysts, the ultrasmall zero-dimensional (0D) ox-GQDs can achieve uniform dispersion on the surface/inner channels of PCNO, as well as intimate contact with PCNO through hydrogen bonding, π-π, and chemical bonding interactions. In contrast with PCNO, the ox-GQDs/PCNO composite photocatalysts possessed improved light-harvesting ability, higher charge-transfer efficiency, enhanced photooxidation capacity, and increased amounts of reactive species due to the upconversion properties, strong electron capturing ability, and peroxidase-like activity of the ox-GQDs. Therefore, the visible-light photocatalytic degradation and disinfection performances of the ox-GQDs/PCNO composite were significantly enhanced. Remarkably, the composite with a 0.2 wt.% deposited amount of ox-GQDs (ox-GQDs-0.2%/PCNO) exhibited optimum amaranth photodegradation activity, with a corresponding rate about 3.1 times as high as that of PCNO. In addition, ox-GQDs-0.2%/PCNO could inactivate about 99.6% of Escherichia coli (E. coli) cells after 4 h of visible light irradiation, whereas only~31.9% of E. coli cells were killed by PCNO. Furthermore, h+,·O2-, and·OH were determined to be the reactive species generated in the photocatalytic process of the ox-GQDs/PCNO system; these species can thoroughly mineralize azo dyes and effectively inactivate pathogenic bacteria.

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Ionization of a covalent organic framework for catalyzing the cycloaddition reaction between epoxides and carbon dioxide Yan Zhang, Hui Hu, Jia Ju, Qianqian Yan, Vasanthakumar Arumugam, Xuechao Jing, Huaqiang Cai, Yanan Gao 2020, 41 (3):  485-493.  DOI: 10.1016/S1872-2067(19)63487-X Abstract ( 126 )   [Full Text(HTML)] () PDF (1593KB) ( 407 )   Covalent organic frameworks (COFs), with two dimensional (2D-) or three dimensional (3D-) structures, have accessible open channels or nanopores, with uniform sizes ranging from angstroms to nanometers and have emerged as an excellent and promising platform for designing catalysts or catalyst carriers. Herein, a 2D-COF grafted with a 1-alkyl-3-methylimidazolium-based ionic liquid (AMIMBr@H2P-DHPh COF) on the channel walls was synthesized and utilized as a highly efficient heterogeneous catalyst for the chemical fixation of CO2 via a reaction with epoxides under solvent-free and co-catalyst-free conditions. The as-synthesized AMIMBr@H2P-DHPh COF shows excellent catalytic activity in promoting the cycloaddition reactions between epoxide and CO2; the excellent catalytic activity was maintained for up to five cycles. Advantages like high porosity, functional versatility, easy modification of COFs, and high catalytic activity of ionic liquids, have been realized in a single material.

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Selective oxidation of glycerol with oxygen in base-free solution over N-doped-carbon-supported Sb@PtSb2 hybrid Lihua Yang, Tianqu He, Chujun Lai, Ping Chen, Zhaoyin Hou 2020, 41 (3):  494-502.  DOI: 10.1016/S1872-2067(19)63476-5 Abstract ( 85 )   [Full Text(HTML)] () PDF (1697KB) ( 267 )   Selective oxidation of glycerol with molecular oxygen in base-free aqueous solutions has become a hot topic, as the rapidly increasing production of biodiesel is creating a surplus of glycerol. In this work, an N-doped-carbon-supported core-shell structured Sb@PtSb2 hybrid catalyst was prepared via a facile synthesis route, in which a mixture of glucose, melamine, and SbCl3 (Sb-NC) was pyrolyzed, then impregnated with Pt by immersion in an aqueous solution of H2PtCl6, and further treated in hydrogen flow. Characterization of the catalyst products indicated that introducing SbCl3 can increase the surface area of the binary glucose + melamine pyrolyzed support (NC), and Sb@PtSb2 hybrids could be formed on the surface of an Sb-NC support during hydrogen treatment at 700℃. It was found that the Sb@PtSb2/NC catalyst was more active for the selective oxidation of glycerol in a base-free aqueous solution than Sb-free NC-supported Pt (Pt/NC). Further characterization also indicated that the promising performance of Sb@PtSb2/NC might be attributed to its enhanced oxygen activation.

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2D/2D type-II Cu2ZnSnS4/Bi2WO6 heterojunctions to promote visible-light-driven photo-Fenton catalytic activity Li Guo, Kailai Zhang, Xuanxuan Han, Qiang Zhao, Yuanyuan Zhang, Mian Qi, Danjun Wang, Feng Fu 2020, 41 (3):  503-513.  DOI: 10.1016/S1872-2067(19)63524-2 Abstract ( 69 )   [Full Text(HTML)] () PDF (1681KB) ( 307 )   In this work, a set of novel Cu2ZnSnS4/Bi2WO6 (CZTS/BWO) two-dimensional (2D)/two-dimensional (2D) type-II heterojunctions with different CZTS weight ratios (1%, 2%, and 5%) were successfully synthesized via a brief secondary solvothermal process. The successful formation of the heterojunctions was affirmed by characterization methods such as X-ray photoelectron spectroscopy and high-resolution transmission electron microscopy. The photocatalytic activity results showed that the prepared CZTS/BWO heterojunctions had excellent photocatalytic behaviors for organic degradation, especially when the mass fraction of CZTS with respect to BWO in the composite was 2%. Moreover, the addition of hydrogen peroxide (H2O2) could further improve the dye and antibiotic degradation efficiencies. The reinforced photocatalytic and photo-Fenton degradation performance were primarily attributable to the introduction of BWO, which afforded increased active sites, expanded the solar spectral response range, and accelerated the cycle of Cu(II)/Cu(I); after four cycling times, its catalytic activity did not decrease significantly. In addition, reasonable hypotheses of the photocatalytic and photo-Fenton catalytic mechanisms were formulated. This study is expected to provide a visual approach for designing a novel photo-Fenton catalyst to jointly utilize the photocatalytic and Fenton activities, which can be better applied to the purification of residual organics in wastewater.

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Co-MOF as an electron donor for promoting visible-light photoactivities of g-C3N4 nanosheets for CO2 reduction Qiuyu Chen, Sijia Li, Hongyi Xu, Guofeng Wang, Yang Qu, Peifen Zhu, Dingsheng Wang 2020, 41 (3):  514-523.  DOI: 10.1016/S1872-2067(19)63497-2 Abstract ( 131 )   [Full Text(HTML)] () PDF (1175KB) ( 467 )   A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride (g-C3N4) nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework (MOF) is proposed in this study. Specifically, Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital (LUMO) to the conduction band of g-C3N4 to facilitate charge separation. As expected, the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities. The CO production rate of 6.75 µmol g-1 h-1 and CH4 evolution rate of 5.47 µmol g-1 h-1 are obtained, which are approximately 2 times those obtained with the original g-C3N4 under the same conditions. Based on a series of analyses, it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation, which improves the photocatalytic activity of g-C3N4 to a higher level. In particular, the hydroxyl radical (·OH) experiment was operated under 590 nm (single-wavelength) irradiation, which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4. This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.

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On the mechanism of H2 activation over single-atom catalyst: An understanding of Pt1/WOx in the hydrogenolysis reaction Maoxiang Zhou, Man Yang, Xiaofeng Yang, Xiaochen Zhao, Lei Sun, Weiqiao Deng, Aiqin Wang, Jun Li, Tao Zhang 2020, 41 (3):  524-532.  DOI: 10.1016/S1872-2067(19)63517-5 Abstract ( 247 )   [Full Text(HTML)] () PDF (3488KB) ( 482 )   Supporting Information Owing to the atomic dispersion of active sites via electronic interaction with supports, single-atom catalysts (SACs) grant maximum utilization of metals with unique activity and/or selectivity in various catalytic processes. However, the stability of single atoms under oxygen-poor conditions, and the mechanism of hydrogen activation on SACs remain elusive. Here, through a combination of theoretical calculation and experiments, the stabilization of metal single atoms on tungsten oxide and its catalytic properties in H2 activation are investigated. Our calculation results indicate that the oxygen defects on the WO3(001) surface play a vital role in the stabilization of single metal atoms through electron transfer from the oxygen vacancies to the metal atoms. In comparison with Pd and Au, Pt single atoms possess greatly enhanced stability on the WOx(001) surface and carry negative charge, facilitating the dissociation of H2 to metal-H species (Hδ-) via homolytic cleavage of H2 similar to that occurring in metal ensembles. More importantly, the facile diffusion of Pt-H to the WOx support results in the formation of Brønsted acid sites (Hδ+), imparting bifunctionality to Pt1/WOx. The dynamic formation of Brønsted acid sites in hydrogen atmosphere proved to be the key to chemoselective hydrogenolysis of glycerol into 1,3-propanediol, which was experimentally demonstrated on the Pt1/WOx catalyst.