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Chinese Journal of Chemical Physics 2017年第3期30卷 333-338,I0002页

作者：姬丽丽李欢张伟孙松高琛鲍骏马运生中国科学技术大学化学物理系合肥230026 中国科学技术大学国家同步辐射实验室合肥230029

A series of carbon nanotubes-supported K-Co-Mo catalysts were prepared by a sol-gel method combined with incipient wetness impregnation. The catalyst structures were characterized by X-ray diffraction, N2 adsorption-desorption, transmission electron microscopy and H2-TPD, and its catalytic performance toward the synthesis of higher alcohols from syngas was investigated. The as-prepared catalyst particles had a low crystallization degree and high dispersion on the outer and inner surface of CNTs. The uniform mesoporous structure of CNTs increased the diffusion rate of reactants and products, thus promoting the reaction conversion. Furthermore, the incorporation of CNTs support led to a high capability of hydrogen absorption and spillover and promoted the formation of alkyl group, which served as the key intermediate for the alcohol formation and carbon chain growth. Benefiting from these characteristics, the CNTs supported Mo-based catalyst showed the excellent catalytic performance for the higher alcohols synthesis as compared to the unsupported catalyst and activated carbon supported catalyst.

关键词： CO hydrogenation Higher alcohol synthesis Mo-based catalyst CNTs support

Nanosheet-structured K–Co–MoS_2 catalyst for the higher alcohol synthesis from syngas: Synthesis and activation

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Journal of Energy Chemistry 2019年第3期28卷 57-62页

作者： Huan Li Wei Zhang Yinyin Wang Meiling Shui Song Sun Jun Bao Chen Gao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials University of Science and Technology of China CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China

The nanosheets structured K–Co–MoS_2 catalyst was prepared through a one-step hydrothermal synthesis combined with the wetness impregnation. The fresh catalyst has a high dispersion of Co–Mo–S active phase and no Co_9S_8 is found. The pure H_2 activated catalyst shows a higher intrinsic activity, especially the C_(2+) OH selectivity for the higher alcohol synthesis compared to the one activated by 5% H_2/N_2 atmosphere. The reason is attributed to that the pure H_2 activation more effectively suppresses the formation of Co_9S_8 and stabilizes the Co–Mo–S active phase during the reaction due to the formation of SH species.

关键词： Syngas Higher alcohol synthesis Mo-based catalyst Co–Mo–S phase

Surface Modification of (001) Facets Dominated TiO2 with Ozone for Adsorption and Photocatalytic Degradation of Gaseous Toluene

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Chinese Journal of Chemical Physics 2019年第5期32卷 611-619页

作者： Yue Yang Zhi-yu Wang Fan Zhang Yi Fan Jing-jing Dong Song Sun Chen Gao Jun Bao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes University of Science and Technology of China Hefei 230029 China Beijing Advanced Innovation Center for Big Data and Brain Computing Beihang University Beijing 100191 China School of Chemistry and Chemical Engineering Anhui University Hefei 230601 China Beijing Advanced Sciences and Innovation center Chinese Academy of Sciences Beijing 101407 China

This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated（001） facets for toluene *** performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mechanism were established by a combination of various characterization methods, in situ diffuse reflectance infrared fourier transform spectroscopy, and density functional theory *** surface modification with ozone can significantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5 c-Ti sites on（001）facets act as the adsorption sites for ozone. The formed Ti–O bonds reacted with H2O to generate a large amount of isolated Ti5 c-OH which act as the adsorption sites for toluene,and thus significantly increase the adsorption capacity for toluene. The outstanding photocatalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH·radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.

关键词： Ozone modification (001) Facets Toluene degradation TiO2 In situ diffuse reflectance infrared fourier transform spectroscopy

Direct Z-scheme CdS-CdS Nanorod Arrays Photoanode: Synthesis,Characterization and Photoelectrochemical Performance

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Chinese Journal of Chemical Physics 2019年第6期32卷 715-720,I0003,I0025-I0031页

作者： Yi Fan Zhi-min Song Jing-jing Dong Zhi-yu Wang Yue Yang Xiao-di Zhu Song Sun Chen Gao Jun Bao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy MaterialsUniversity of Science and Technology of ChinaHefei 230029China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601China Beijing Advanced Sciences and Innovation Center Chinese Academy of SciencesBeijing 101407China

Direct Z-scheme CdO-CdS 1-dimensional nanorod arrays were constructed through a facile and simple hydrothermal process. The structure, morphology, photoelectrochemical properties and H2 evolution activity of this catalyst were investigated systematically. The morphology of the obtained nanorod is a regular hexagonal prism with 100-200 nm in diameter. The calcination temperature and time were optimized carefully to achieve the highest photoelectrochemical performance. The as-fabricated hybrid system achieved a photocurrent density up to 6.5 mA/cm2 and H2 evolution rate of 240 μmol·cm-2·h-1 at 0 V vs. Ag/AgCl, which is about 2-fold higher than that of the bare CdS nanorod arrays. The PEC performance exceeds those previously reported similar systems. A direct Z-scheme photocatalytic mechanism was proposed based on the structure and photoelectrochemical performance characterization results, which can well explain the high separation efficiency of photoinduced carriers and the excellent redox ability.

关键词： Direct Z-scheme CdO-CdS One-Dimensional nanorod arrays PEC performance H2 evolution rate

Accelerating C_(2+)alcohols synthesis from syngas by simultaneous optimizations of CO dissociation and chain growth over CuCo alloy catalyst

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Chinese Chemical Letters 2021年第7期32卷 2203-2206页

作者： Meiling Shui Chao Huang Peiyu Ma Wenjie Li Qun He Wenlong Wu Yisheng Tan Jun Bao National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Hefei National Laboratory for Physical Sciences at the Microscale Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of SciencesKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China

With regard to the reaction of higheralcohol synthesis(HAS),the optimizations of activity and selectivity towards C_(2+)alcohol are restricted by the improper equilibrium in two different CO activation pathways and chain growth ***,we find that delibrately controlling the compositions of catalysts is an effective strategy to achieve the equilibrium of CO activation pathways and promote the chain *** a result,the optimized Cu_(0.25)Co_(0.75) alloy catalyst can achieve a large proportion of higher alcohol in alcohol products(C_(2+)OH/MeOH=4.40),together with high CO conversion of 71.27%and space-time-yield of 147.65 g kg^(-1) h^(-1).The mechanistic studies suggest that the good performance of Cu_(0.25)Co_(0.75) catalyst is attributed to the synergistic effect between alloyed Cu and Co.

关键词： CuCo alloy Syngas C_(2+)alcohols CO activation Synergistic effect

K-Co-Mo/CNTs催化剂合成低碳醇性能研究（英文）

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Chinese Journal of Chemical Physics 2017年第3期 333-338页

作者：姬丽丽李欢张伟孙松高琛鲍骏马运生中国科学技术大学化学物理系中国科学技术大学国家同步辐射实验室

采用溶胶-凝胶法结合等体积浸渍法制备了一系列不同Mo负载量的K-Co-Mo/CNTs催化剂.通过X射线衍射、N2等温吸脱附,透射电子显微镜和H2-TPD表征了催化剂结构,并研究了碳纳米管催化剂使用合成气合成低碳醇的催化性能.所制备的催化剂颗粒在C... 详细信息

采用溶胶-凝胶法结合等体积浸渍法制备了一系列不同Mo负载量的K-Co-Mo/CNTs催化剂.通过X射线衍射、N2等温吸脱附,透射电子显微镜和H2-TPD表征了催化剂结构,并研究了碳纳米管催化剂使用合成气合成低碳醇的催化性能.所制备的催化剂颗粒在CNTs载体的外表面和内表面上具有低结晶度和高分散性.CNTs载体的均匀介孔结构增加了反应物和产物的扩散速率,从而促进了反应转化.此外,CNTs载体的引入促进了氢的吸附和活化,而且和解离H物种的相互作用较弱,易于H的溢流,并促进了烷基的形成,烷基是形成醇产物和碳链增长的重要中间体.受益于这些特征,与传统的活性炭催化剂相比,CNTs负载的K-Co-Mo催化剂显示出更加优异的合成醇性能.

关键词： CO加氢低碳醇 Mo基催化剂碳纳米管载体

Visible-light deposition of CrO_(x) cocatalyst on TiO_(2):Cr valence regulation for superior photocatalytic CO_(2)reduction to CH_(4)

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Journal of Energy Chemistry 2022年第1期31卷 103-112,I0004页

作者： Jingjing Dong Yuan Kong Heng Cao Zhiyu Wang Zhirong Zhang Lidong Zhang Song Sun Chen Gao Xiaodi Zhu Jun Bao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy MaterialsUniversity of Science and Technology of ChinaHefei 230029AnhuiChina Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics Synergetic Innovation Center of Quantum Information and Quantum PhysicsUniversity of Science and Technology of ChinaHefei 230026AnhuiChina School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601AnhuiChina School of Physical Science University of Chinese Academy of SciencesBeijing 100049China

Photodeposition is widely adopted for implanting metal/metal oxide cocatalysts on ***,it is prerequisite that the photon energy should be sufficient to excite the host ***,we report a lower-energy irradiation powered deposition strategy for implanting CrO_(x) cocatalyst on TiO_(2).Excitingly,CrO_(x)-400 implanted under visible-light irradiation significantly promotes the CH4 evolution rate on TiO_(2)to 8.4μmolg·^(-1)h^(-1) with selectivity of98%from photocatalytic CO_(2)reduction,which is 15 times of that on CrO_(x)-200 implanted under UV-visible-light ***,CrO_(x)-400 is identified to be composed of higher valence Cr species compared to CrO_(x)-*** valence states regulation of Cr species is indicated to provide more active sites for CO_(2) adsorption/activation and to modulate the reaction mechanism from single Cr site to Cr-Cr dual sites,thus endowing the superior CH_(4)*** work demonstrates an alternative strategy for constructing efficient metal oxides cocatalysts on wide bandgap semiconductor.

关键词： Valence states regulation CrO_(x)cocatalyst Lower-energy irradiation Photocatalytic CO_(2)reduction High CH_(4)selectivity

Enhance the activity of multi-carbon products for Cu via P doping towards CO_(2) reduction

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Science China Chemistry 2021年第7期64卷 1096-1102页

作者： Xiangdong Kong Cheng Wang Han Zheng Zhigang Geng Jun Bao Jie Zeng Hefei National Laboratory for Physical Sciences at the Microscale Key La boratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of SciencesKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China

Electronic structure engineering is a powerful method to tailor the behavior of adsorbed intermediates on the surface of catalysts,thus regulating catalytic activity towards CO_(2)***,we prepared a series of P-doped Cu catalysts for CO_(2)electroreduction into multi-carbon(C_(2+))products by regulating the surface electronic structure of *** introduction of P could stabilize the surface Cu^(δ+)species,enhancing the activity for C_(2+)products via adjusting the adsorbed strength of the CO intermediates(~*CO).When the molar ratio of P to Cu was 8.3%,the catalyst exhibited a Faradaic efficiency of 64%for C_(2+)products,which was 1.9 times as high as that(33%)for Cu catalysts at the applied current density of 210 m A cm^(-2).Notably,at the applied current density of 300 mA cm^(-2),the P-doped Cu catalyst with the molar ratio of P to Cu of 8.3%exhibited the highest partial current density for C_(2+)products of 176 mA cm^(-2),whereas the partial current density for C_(2+)products over the Cu catalyst was only 84 mA cm^(-2).Mechanistic studies revealed that modulating the molar ratios of P to Cu regulated the adsorbed strength of~*CO.A moderate adsorbed strength of *CO induced by appropriate P doping was responsible for the facilitated C–C coupling process.

关键词： P-doped Cu catalysts C^(2+)products ~*CO adsorption CO_(2)electroreduction

Constructing subtle grain boundaries on Au sheets for enhanced CO2 photoreduction

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Science China Chemistry 2020年第12期63卷 1705-1710页

作者： Xu Li Tingting Zheng Lan Zhang Songtao Zhao Yinuo Chen Miaojin Wei Chunyan Shang Jun Bao Jie Zeng Hefei National Laboratory for Physical Sciences at the Microscale National Synchrotron Radiation LaboratoryCAS Key Laboratory of Strongly-Coupled Quantum Matter PhysicsKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042China

Photocatalytic reduction of CO2 into value-added products is a promising strategy for mitigating environmental and energy problems ***,we developed Au sheets with subtle grain boundaries on ultrathin Ni(OH)2 nanosheets as efficient photocatalysts for CO2 *** to mechanistic studies,grain boundaries on the Au sheets served as electron trapping sites which enabled the optimization of electron-hole ***,grain boundaries perturbed electron distribution,which assisted in stabilizing CO2^δ- and HCOO^* *** a result,the unique hybrid structure achieved a high rate of 75.2μmol g^-1h^-1 for CO2 *** work demonstrates the importance of defect engineering in designing active photocatalysts and also provides insight into development of related photo-energy conversion schemes.

关键词： Au sheet grain boundary Ni(OH)2 nanosheet CO2 photoreduction

Directing in-situ self-optimization of single-atom catalysts for improved oxygen evolution

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Journal of Energy Chemistry 2023年第5期80卷 284-290,I0007页

作者： Peiyu Ma Chen Feng Huihuang Chen Jiawei Xue Xinlong Ma Heng Cao Dongdi Wang Ming Zuo Ruyang Wang Xilan Ding Shiming Zhou Zhirong Zhang Jie Zeng Jun Bao Hefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of SciencesKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei230026AnhuiChina National Synchrotron Radiation Laboratory iChEM(Collaborative Innovation Center of Chemistry for Energy Materials)University of Science and Technology of ChinaHefei 230026AnhuiChina

The demand for clean and sustainable energy has encouraged the production of hydrogen from water *** overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution ***,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction ***,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized *** introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single ***,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated *** revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/*** results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.

关键词： Electrocatalysis Single-Atom Catalysis Self-Optimization Oxygen Evolution