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Chinese Chemical Letters 2020年第1期31卷 231-234页

作者： Yunong Li Lei Wang Jingxiang Low Di Wu Canyu Hu Wenbin Jiang Jun Ma Chengming Wang Ran Long Li Song Hangxun Xu Yujie Xiong Hefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) School of Chemistry and Materials Science National Synchrotron Radiation Laboratory University of Science and Technology of China

Efficient catalytic system with low energy consumption exhibits increasing importance due to the upcoming energy *** this situation,it should be an admirable strategy for reducing energy input by effectively utilizing incident solar energy as a heat source during catalytic ***,aza-fused7 r-conjugated microporous polymer(aza-CMP)with broad light absorption and high photothermal conversion efficiency was synthesized and utilized as a support for bimetallic AuPd nanocatalysts in light-driven benzyl alcohol *** AuPd nanoparticles anchored on aza-CMP(aza-CM P/Au_xPdy)exhibited excellent catalytic performance for benzyl alcohol oxidation under 50 mW/cm^2 light *** improved catalytic performance by the aza-CMP/Au_xPdy is attributed to the unique photothermal effect induced by aza-CMP,which can promote the catalytic benzyl alcohol oxidation occurring at Au *** work presents a novel approach to effectively utilize solar energy for conventional catalytic reactions through photothermal effect.

关键词： Aza-CMP AuPd Photothermal benzyl alcohol oxidation Catalysis

Catalytic Performance of Graphite Oxide Supported Au Nanoparticles in Aerobic oxidation of benzyl alcohol： Support Effect

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Chinese Journal of Chemical Physics 2017年第1期30卷 90-96,I0002页

作者： Yu-jia Huo Fan-fan Yao Yun-sheng Ma Department of Chemical Physics University of Science and Technology of China Hefei 230026 China

Various Au/GO catalysts were prepared by depositing Au nanoparticles on thermally- and chemically-treated graphite oxide （GO） supports using a sol-immobilization method. The surface chemistry and structure of GO supports were characterized by a series of analytical techniques including X-ray photoelectron spectroscopy, temperature-programmed desorption and Raman spectroscopy. The results show that thermal and chemical treatments have large influence on the presence of surface oxygenated groups and the crystalline structure of GO supports. A strong support effect was observed on the catalytic activity of Au/GO catalysts in the liquid phase aerobic oxidation of benzyl alcohol. Compared to the amount and the type of surface oxygen functional groups, the ordered structure of GO supports may play a more important role in determining the catalytic performance of Au/GO catalysts.

关键词： Gold nanoparticles Graphite oxide Catalyst benzyl alcohol oxidation X-ray photoelectron spectroscopy Temperature-programmed desorption Raman

Enhanced water-induced effects enabled by alkali-stabilized Pd-OH_(x) species for oxidation of benzyl alcohol

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Chinese Chemical Letters 2023年第6期34卷 236-241页

作者： Qianbing Wei Chang Yu Yongwen Ren Lin Ni Dongming Liu Lin Chen Hongling Huang Yingnan Han Junting Dong Jieshan Qiu State Key Lab of Fine Chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024China College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

The water promotion effects,where water can provide a solution-mediated reaction pathway in various heterogeneous chemical catalysis,have been presented and attracted wide attention recently,yet,the rational design of catalysts with a certain ability of enhancing water-induced reaction process is full of challenges and ***,we show that by incorporating alkali(Na,K)cations as an electronic and/or structural promoter into Pd/rGO-ZnCr_(2)O_(4)(r GO,reduced graphene oxide),the obtained Pd(Na)/rGO-ZnCr_(2)O_(4)as a representative example demonstrates an outstanding benzyl alcohol oxidation activity in the Pickering emulsion system in comparison to the alkali-free *** response experiments of water injection confirm the enhanced activity,and the Na-modified catalyst can further enhance the promotion effects of water on the *** effects of alkali cations for Pd nanoparticles are identified and deciphered by a series of experimental characterizations(XPS,in situ CO-DRIFTS,and CO-TPR coupled with MS),showing that there is abundant-OH on the surface of the catalyst,which is stabilized by the formation of Pd-OH_(x).The alkali-stabilized Pd-OH_(x)is helpful to enhance the waterinduced reaction *** to the results of in situ Raman as well as UV-vis absorption spectra,the Na-modulated Pd(Na)/rGO-ZnCr_(2)O_(4)enables the beneficial characteristics for distorting the benzyl alcohol structure and enhancing the adsorption of benzyl ***,the mechanism for enhanced water promotion effects is rationally *** strategy of alkali cations-modified catalysts can provide a new direction to effectively enhance the chemical reaction involving small molecule water.

关键词： Alkali metals benzyl alcohol oxidation Heterogeneous catalysis Pickering emulsion Water effects

Construction of hierarchical photocatalysts by growing ZnIn_(2)S_(4) nanosheets on Prussian blue analogue-derived bimetallic sulfides for solar co-production of H_(2) and organic chemicals

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Journal of Energy Chemistry 2021年第3期30卷 386-394页

作者： Liangxuan Zhong Baodong Mao Meng Liu Mingyue Liu Yaqiu Sun Yi-Tao Song Zhi-Ming Zhang Tong-Bu Lu Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China Institute for New Energy Materials&Low Carbon Technologies School of Materials Science&EngineeringTianjin University of TechnologyTianjin 300384China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

Exploring highly efficient bifunctional photocatalysts for simultaneous H2 evolution and organic chemical production in pure water represents a green route for sustainable solar energy storage and ***,a facile strategy was explored for preparing a hierarchical porous heterostructure of Fe_(4)Ni_(5)S_(8)@ZnIn_(2)S_(4)(FNS@ZIS)by the in situ growth of ZIS nanosheets on Prussian blue analogue(PBA)-derived bimetallic FNS sulfides.A series of FNS@ZIS hierarchical structures were facilely prepared by adjusting the loading amount(n%)of FNS(n=19,26,and 32 for FNS@ZIS-1-3).These structures can efficiently drive the solar co-production of H_(2) and organic *** optimal co-production was achieved with FNS@ZIS-2,affording a H_(2) evolution rate of 10465μmol·g^(-1)·h^(-1),along with high selectivity for the oxidation of benzyl alcohol to benzaldehyde(>99.9%).The performance was 22 and 31 times higher than that of FNS and ZIS,respectively,and even superior to the state-of-the-art results achieved using various sacrificial *** mechanistic study indicated that the unique hierarchical core/shell architecture can facilitate interfacial charge separation,afford bimetallic synergy,abundant active sites and excellent *** work highlights a simple and efficient method for preparing porous multimetallic hierarchical structures for the solar co-production of organic chemicals and H_(2) fuel.

关键词： Prussian blue analogue Photocatalysis Hydrogen evolution benzyl alcohol oxidation Coordination polymer

Optimizing geometric configuration of single Zn-N_(4) sites for boosting reciprocal transformation between aromatic alcohols and aldehydes

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Nano Research 2023年第7期16卷 9132-9141页

作者： Shengjie Wei Yucheng Jin Chunlin Lv Chao Lian Zheng Chen Xiao Liang Qinghua Zhang Xin Chen Dongdong Qi Zhi Li School of Materials Science and Engineering Nankai UniversityTianjin 300350China Department of Chemistry Tsinghua UniversityBeijing 100084China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing 100083China School of Pharmacy and Center on Translational Neuroscience Minzu University of ChinaBeijing 100081China Department of Chemistry School of ScienceBeijing Jiaotong UniversityBeijing 100091China School of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Beijing Advanced Innovation Center for Materials Genome Engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083China College of Chemistry Beijing Normal UniversityBeijing 100875China

It is significant to optimize geometric configuration of metal catalytic sites and boost their catalytic ***,we synthesized isolated single Zn-N_(4)sites on N-doped carbon(Zn-CN)by pyrolyzing zeolite imidazole framework-8(ZIF-8)at different *** the reciprocal transformation between benzyl alcohol and benzaldehyde,the catalytic activities of Zn-CN catalysts exhibited a volcano-like trend as the pyrolysis temperatures *** optimal catalyst was Zn-CN-900,with outstanding catalytic activity exceeding commercial 20 wt.%Pd/C and 20 wt.%Pt/C,promising to substitute the noble metalbased catalysts.X-ray absorption near-edge structure(XANES)measurements and density functional theory(DFT)calculation revealed the gradual transformation from tetrahedral ZnN_(4)sites of ZIF-8 into planar ZnN_(4)sites above 700℃,with the maximum planar ZnN_(4)sites in *** stronger adsorption between reactants and planar ZnN_(4)sites facilitated the activation of reactants compared with tetrahedral ZnN_(4)*** work will provide valuable insight into rational design of efficient catalysts by optimizing geometric configuration of catalytic sites.

关键词： geometric configuration single Zn-N_(4)sites benzyl alcohol oxidation hydrogen transfer reaction

Ferric acetylacetonate/covalent organic framework composite for high performance photocatalytic oxidation

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Green Energy & Environment 2022年第6期7卷 1281-1288页

作者： Mingzhao Xu Lifei Liu Jianling Zhang Fanyu Zhang Gang Chen Qiang Wan Yufei Sha Xiuyan Cheng Zhuizhui Su Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemistry and Chemical Engineering University of Chinese Academy of SciencesBeijing100049China School of Chemical Sciences University of Chinese Academy of SciencesPhysical Science LaboratoryHuairou National ComprehensiveScience CenterBeijing100190China

Ferric acetylacetonate/covalent organic framework(Fe(acac)_(3)/COF)composite was synthesized by interfacial polymerization method at room *** crystal structure,morphology and porosity property of the composite were characterized by X-ray diffraction,scanning electron microscope,transmission electron microscope and nitrogen *** interaction between Fe(acac)_(3) and COF was investigated by Fourier transform infrared spectra and X-ray photoelectron *** Fe(acac)_(3)/COF composite was used as a photocatalyst for the oxidation of benzyl alcohol under mild *** exhibits high activity and selectivity for the reaction,of which the mechanism was investigated by determining its photoelectric *** Fe(acac)_(3)/COF catalyst developed in this work has application potential in other photocatalytic reactions.

关键词： Covalent organic framework Photocatalysis Hybrid catalyst benzyl alcohol oxidation Interfacial polymerization

Noble-metal-free plasmonic MoO_(3-x)-based S-scheme heterojunction for photocatalytic dehydrogenation of benzyl alcohol to storable H2 fuel and benzaldehyde

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Chinese Journal of Catalysis 2022年第10期43卷 2665-2677页

作者： Yingcong Wei Qiqi Zhang Ying Zhou Xiongfeng Ma Lele Wang Yanjie Wang Rongjian Sa Jinlin Long Xianzhi Fu Rusheng Yuan State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350108FujianChina School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina School of Environment&Civil Engineering Dongguan University of TechnologyDongguan 523808GuangdongChina Institute of Oceanography Ocean CollegeMinjiang UniversityFuzhou 350108FujianChina

Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical ***,for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol(BA)into benzaldehydes(BAD)and H_(2),a novel localized surface plasmon resonance(LSPR)enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_(3-x) as oxidation semiconductor and Zn_(0.1)Cd_(0.9)S as reduction *** photoredox system of Zn_(0.1)Cd_(0.9)S/MoO_(3-x) displayed an unconventional reaction model,in which the BA served as both electron donor and *** S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation ***,due to the LSPR effect of MoO_(3-x) nanosheets,Zn_(0.1)Cd_(0.9)S/MoO_(3-x) photocatalysts exhibited strong absorption in the region of full solar ***,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite generated H_(2) and BAD simultaneously via selective oxidation of BA with high production(34.38 and 33.83 mmol×g^(–1) for H_(2) and BAD,respectively)upon full solar *** under NIR light irradiation,the H_(2) production rate could up to 94.5 mmol×g^(–1)×h^(–1).In addition,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite displayed effective photocatalytic H_(2) evolution rate up to 149.2 mmol×g^(–1)×h^(–1) from water,which was approximate 6 times that of pure Zn_(0.1)Cd_(0.9)*** work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.

关键词： Zn_(0.1)Cd_(0.9)S/MoO_(3-x)S-scheme heterojunction Localized surface plasmon resonance benzyl alcohol oxidation Hydrogen generation Full-spectrum light response

金属相1T-MoS_(2)/ZnIn_(2)S_(4)异质结调控电荷传输从而促进光催化氧化还原反应

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Science China Materials 2024年第2期67卷 532-540页

作者：张洪文姚雪山巍刘玥唐华 School of Environmental Science and Engineering Qingdao UniversityQingdao 266071China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China

近年来,光催化产氢与有机物氧化的偶联反应备受关注,如何设计高效双功能光催化剂实现偶联反应成为研究重点.在众多光催化剂中,ZnIn_(2)S_(4)以其优异的可见光吸收能力、本征的极化电场以及较强的氧化还原能力成为双功能催化剂的热点备... 详细信息

近年来,光催化产氢与有机物氧化的偶联反应备受关注,如何设计高效双功能光催化剂实现偶联反应成为研究重点.在众多光催化剂中,ZnIn_(2)S_(4)以其优异的可见光吸收能力、本征的极化电场以及较强的氧化还原能力成为双功能催化剂的热点备选材料.然而,电子空穴分离效率低以及光生电子空穴复合率高的问题限制了ZnIn_(2)S_(4)光电转化效率的进一步提高.针对这一问题,我们采用了具有较高导电性和独特结构的金属相1T-MoS_(2)作为助催化剂与花状ZnIn_(2)S_(4)复合形成“海胆状”的1T-MoS_(2)/ZnIn_(2)S_(4)欧姆结复合材料.理论计算结合XPS数据揭示了欧姆结与内建电场的形成,一系列光谱表征表明由欧姆结所形成的强内建电场促进了ZnIn_(2)S_(4)体内光生电子快速向1T-MoS_(2)转移,同时活性测试与EPR表征证明了苯甲醇的氧化反应可以作为光生空穴的有效捕获剂.最终,1T-MoS_(2)/ZnIn_(2)S_(4)复合光催化剂实现了4.6倍光催化性能的提高,420 nm波长下表光量子效率达6.75%.本项工作通过精确调节电荷转移机制,实现了ZnIn_(2)S_(4)双功能催化剂光电效率的进一步提高,为光催化剂载流子调控设计提供了新思路.

关键词： metallic 1T-MoS_(2) heterojunction photocatalyst photocatalytic hydrogen evolution benzyl alcohol oxidation guiding charge migration