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Bi-, Y-Codoped TiO2 for Carbon Dioxide Photocatalytic Reduction to formic acid under Visible Light Irradiation

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Chinese Journal of Chemistry 2018年第6期36卷 538-544页

作者： Pengju Du Tongming Su Xuan Luo Xiantai Zhou Zuzeng Qin Hongbing Ji Jianhua Chen School of Chemistry and Chemical Engineering Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Tech- nology Guangxi University Nanning Guangxi 530004 China School of Chemistry Sun Yat-sen University Guangzhou Guangdong 510275 China College of Resources Environment and Materials Guangxi University Nanning Guangxi 530004 China

Bi- and Y-codoped TiO2 photocatalysts were synthesized through a sol-gel method, and they were applied in the photocatalytic reduction of CO2 to formic acid under visible light irradiation. The results revealed that, after doping Bi and Y, the surface area of TiO2 was increased from 5.4 to 93.1 m2/g when the mole fractions of doping Bi and Y were 1.0% and 0.5%, respectively, and the lattice structures of the photocatalysts changed and the oxygen vacancies on the surface of the photocatalysts formed, which would act as the electron capture centers and slow down the recombination of pho- to-induced electron and hole. The photocurrent spectra also proved that the photocatalysts had better electronic transmission capacities. The HCOOH yield in CO2 photocatalytic reduction was 747.82 μmol/gcat by using 1% Bi-0.5% Y-TiO2 as a photocatalyst. The HCOOH yield was 1.17 times higher than that by using 1% Bi-TiO2, and 2.23 times higher than that by using pure TiO2. Furthermore, the 1% Bi-0.5% Y-TiO2 showed the highest apparent quantum efficiency （AQE） of 4.45%.

关键词： bismuth yttrium titanium dioxide photocatalytic reduction carbon dioxide formic acid

Facile Synthesis of Pd-Ni Nanoparticles on Reduced Graphene Oxide under Microwave Irradiation for formic acid Oxidation

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Chinese Journal of Chemistry 2017年第9期35卷 1405-1410页

作者： Miaoyu Li Ruiqin Liu Gaoyi Han Yanni Tian Yunzhen Chang Yaoming Xiao Institute of Molecular Science Key Laboratory of Materials for Energy Conversion and Storage of Shanxi Province Shanxi University Taiyuan Shanxi 030006 China

Pd and PdxNi nanoparticles have been supported on reduced graphene oxide （Pd/rGO and PdxNi/rGO） by using the microwave-assisted heating method in glycol. The morphology, composition and electrochemical performance have been characterized by TEM, XRD, XPS and electrochemical methods. The XRD and XPS results show that there are no PdNi alloy particles formed in PdxNi/rGO and the composites exist mostly in the form of Pd^0 and NiOOH species. The electrochemical results reveal that PdxNi/rGO synthesized from the feeding source of Pd and Ni with an atomic ratio of 4 ： 1 exhibits higher activity, better stability and smaller electron transfer resistance to- ward formic acid electro-oxidation compared with commercial Pd/C, Pd/rGO and other PdxNi/rGO samples. The excellent electrocatalytic performance indicates that the addition of appropriate amount of Ni can greatly enhance the activity and stability of Pd catalysts for formic acid oxidation.

关键词： graphene palladium palladium-nickel formic acid electro-oxidation

Catalytic transfer hydrogenation of biomass-derived furfural to furfuryl alcohol with formic acid as hydrogen donor over CuCs-MCM catalyst

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Chinese Chemical Letters 2021年第3期32卷 1186-1190页

作者： Tao Wang Juan Du Yong Sun Xing Tang Zuo-Jun Wei Xianhai Zeng Shi-Jie Liu Lu Lin Xiamen Key Laboratory of Clean and High-valued Utilization for Biomass College of EnergyXiamen UniversityXiamen 361102China Fujian Engineering and Research Center of Clean and High-valued Technologies for Biomass Xiamen 361102China School of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China Department of Paper and Bioprocess Engineering State University of New York College of Environmental Science and ForestrySyracuseNew York 13210United States State Key Laboratory of Applied Microbiology Southern China Guangdong Provincial Key Laboratory of Microbial Culture Collection and ApplicationGuangdong Open Laboratory of Applied MicrobiologyGuangdong Microbial Culture Collection Center(GDMCC)Guangdong Institute of MicrobiologyGuangdong Academy of SciencesGuangzhou 510070China

Catalytic transfer hydroge nation(CTH)of furfural(FF)to furfu ryl alcohol(FFA)has received great intere st in recent *** rein,Cu-Cs bimetallic supported catalyst,CuCs(2)-MCM,was developed for the CTH of FF to FFA using formic as hydrogen ***(2)-MCM achieved a 99.6%FFA yield at an optimized reaction conditions of 170℃,1 *** species in CuCs(2)-MCM had dual functions in catalytically decomposing formic acid to generate hydrogen and hydrogenating FF to *** doping of Cs made the size of Cu particles smaller and improved the dispersion of the Cu active *** rtantly,the Cs species played a favorable role in enhancing the hydrogenation activity as a promoter by adjusting the surface acidity of Cu species to an appropriate *** analysis showed that surface acidity is the primary factor to affect the catalytic activity of CuCs(2)-MCM.

关键词： Furfural Furfuryl alcohol CuCs(x)-MCM catalysts Catalytic transfer hydrogenation formic acid

Hydrothermal Synthesis and Thermal Analyses of an Infinite Three-dimensional Coordination Polymer Based on formic acid： [Zn（HCOO）2（H2O）2]∞

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Chinese Journal of Chemistry 2006年第6期24卷 745-749页

作者：郭金玉张同来张建国 State Key Laboratory of Explosion Science and Technology at Beijing Institute of Technology Beijing 100081China

The coordination polymer [Zn（HCOO）2（H2O）2]∞ has been synthesized using hydrothermal method and characterized by X-ray single crystal diffraction, elemental analysis, FTIR spectroscopy and TG-DTG analyses. The coordination polymer crystallizes in monoclinic, P21/c space group with crystal parameters of α=0.8688（1） nm, b= 0.7143（6） nm, c=0.9305（2） nm, β=97.61（5）°, V=0.5724（2） nm^3, Z=4, μ（Mo Kα）=42.50 cm^-1. The polymer features with two kinds of zinc centers： one is hexa-coordinated by four water ligands, two oxygen atoms of two formates and the other is coordinated by six oxygen atoms of six formates. By the formates as space linkers, three-dimensional frameworks were formed. Based on thermal analyses, thermal decomposition mechanisms were predicted that at the first step the polymer lost two coordination water molecules and at the second step lost two formates companied by the formation of some kinds of materials.

关键词： coordination polymer formic acid crystal structure thermal analysis

Revealing the true origin of size-dependent Pd/C catalytic behavior towards formic acid decomposition

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Chinese Chemical Letters 2023年第1期34卷 457-460页

作者： Qinglei Meng Xian Wang Meiling Xiao Zhao Jin Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

formic acid decomposition(FAD)is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen *** optimize the catalysts for FAD,efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed ***,such endeavors are highly challenging due to the deeply intermingled effects of electronic structure,particle size,and facets,***,to separately evaluate the respective effects of these factors,a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment *** performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%.However,they showed 252%deviation of site stability,indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst’s life.

关键词： Hydrogen production formic acid Catalyst deactivation Size effect Facets effect

Preparation of Platinum Implanted Glassy Carbon Electrode and Electro-oxidation of formic acid and Formaldehyde

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Chinese Chemical Letters 2000年第1期11卷 71-74页

作者： Cun Zhong ZHANG Jing YANG Xiao Lin LU Zhong Da WU( Department of Chemistry, Beijing Normal University, Beijing 100875) Department of Chemistry Beijing Normal University Beijing 100875 China

The glassy carbon substrates were bombarded with 5 X 10(17) ions/cm(2) of platinum. The surface composition of implanted electrode and concentration-depth profiles of various elements were measured by AES. The chemical state of Pt in glassy carbon electrode implanted with platinum (Pt/GC) was detected by X-ray Photoelectron Spectroscopy (XPS). The electro-oxidation of HCOOH and HCHO have been investigated on Pt/CC and smooth Pt electrodes. The results show that the platinum implanted into glassy carbon is much more active than the smooth platinum metal for electro-oxidation of HCOOH and HCHO.

关键词： ion implantation electro-oxidation formic acid formaldehyde

Air-tolerant direct reductive N-methylation of amines using formic acid via simple inorganic base catalysis

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Chinese Chemical Letters 2020年第1期31卷 111-114页

作者： Yan Huang Wei Deng Bo-Lin Lin School of Chemical and Environmental Engineering Shanghai Institute of TechnologyShanghai 201418China School of Technology and Physical Science ShanghaiTech UniversityShanghai 201210China

The construction of N-methyl amine moieties is an important reaction that has found numerous *** of new methylation agents that are more environmentally benign than classical agents,such as iodomethane and methyl sulfate,is still highly ***,we report a convenient protocol for direct reductive N-methylation of amines using formic acid as the methylation agent via simple inorganic base *** present protocol operates under transition-metal-free and air-tolerant *** the catalyst,K2 HPO4,and the reductant,polymethylhydrosiloxane(PMHS),are cheap and easily separable from the crude reaction product *** investigations suggest that the reaction occur through the formation of an acetal inte rmediate followed by the C-N bond formation.

关键词： Air tolerant N-Methylation formic acid Simple inorganic bas Transition-metal-free

Exceptional activity of amino-modified rGO-immobilized PdAu nanoclusters for visible light-promoted dehydrogenation of formic acid

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Chinese Chemical Letters 2024年第7期35卷 428-432页

作者： Yiyue Ding Qiuxiang Zhang Lei Zhang Qilu Yao Gang Feng Zhang-Hui Lu Key Laboratory of Energy Catalysis and Conversion of Nanchang College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022China School of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330031China

formic acid(FA),which is obtainable through CO_(2)hydrogenation with green hydrogen or biomass conversion,has been used as a prospective liquid organic hydrogen carrier(LOHC)because of the abundant advantages of renewability,wide availability,stability,and high volumetric capacity(53 g H_(2)/L).The development of highly efficient catalytic systems to achieve enhanced catalytic activity is attractive but still ***,ultrafine and highly dispersed PdAu nanoclusters(NCs)anchored on amino-modified reduced graphene oxide(ArGO)were successfully synthesized via a facile impregnation-reduction method and applied as a catalyst toward formic acid dehydrogenation(FAD).Benefiting from the promoting effect of amino groups,the strain and ligand effect in the alloy,and the Mott–Schottky effect between PdAu NCs and ArGO,the resultant PdAu/ArGO affords an ultrahigh activity under visible light irradiation with an exceptional turnover frequency value of 10,699.5 h^(-1)at 298 K without any additives,more than 2.6times improvement than that under dark,which is the highest among all reported catalysts under the same *** study provides a green and convenient strategy for developing more efficient and sustainable FAD catalysts and promotes the effective utilization of FA as a prospective renewable LOHC.

关键词： Visible-light-enhanced Hydrogen production formic acid Pd-Au Heterogeneous catalyst

High faradic efficiency of CO_(2) conversion to formic acid catalyzed by Cu_(2)O hollow‑dices

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Carbon Neutrality 2022年第1期1卷 92-98页

作者： Jing Li Chen Meng Jingkun Gu Honglin Wang Ruoyun Dai Haozhi Sha Hongwei Zhu State Key Laboratory of Solid Waste Reuse for Building Materials Beijing Building Materials Academy of Sciences Research100041 BeijingChina State Key Lab of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua University100084 BeijingChina Department of Chemistry Tsinghua University100084 BeijingChina Key Lab of Advanced Materials of Ministry of Education of China National Center for Electron Microscopy in BeijingTsinghua University100084 BeijingChina.

Cu_(2)O has been intensively studied as an efficient catalyst for CO_(2) reduction reaction(CO_(2)RR).By various methods for fine-tuning the morphology and surface modification,high selectivity and activity of different products can be ***,we report a novel Cu_(2)O nanostructure design by facet-controlled etching,during which the catalyst structure switched from a cuboctahedron architecture to a hollow dice-like *** as-etched catalysts exhibit a high Faradic efficiency of formic acid,reaching 75.1% at a low potential of -1.0 *** characterizations indicate that the performance enhancement is attributed to the increased oxygen vacancies induced by the etching *** Cu_(2)O nanostructure design provides a new approach for high-efficiency catalysts for formic acid production at low potentials.

关键词： CO_(2)reduction Cu_(2)O formic acid Facet-controlled etching Oxygen vacancy