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Chinese Chemical Letters 2019年第12期30卷 2309-2312页

作者： Ge Huang Yue Wang tianfu liu Fujian Institute of Research on the Structure of Matter State Key Laboratory of Structural ChemistryChinese Academy of SciencesFuzhou 350002China College of Biological and Chemical Engineering Chongqing University of EducationChongqing 400067China

A stable hierarchical porous metal-organic framework PCN-56 with abundant Lewis acid sites(denoted as Defective-PCN-56) was synthesized by the low-temperature synthesis-induced defect formation *** existence of mesopore in structure was confirmed by N2 sorption isotherm and the successful encapsulation of large dye *** Defective-PCN-56 has higher loading capacity toward anti-cancer drug Doxo compared with that of "nearly ideal-crystal"(denoted as Ideal-PCN-56)synthesized at high temperature,showing potential application as drug *** low-temperature synthesis-induced defect formation strategy presented here provides a new and facile way to synthesize stable MOFs with the combination of intrinsic micropore and additional mesopore as well as abundant Lewis acid sites.

关键词： Low-temperature induced Defect formation strategy Stable MOFs Hierarchical porous MOFs Lewis acid sites

High-throughput mechanistic study of highly selective hydrogen-bonded organic frameworks for electrochemical nitrate reduction to ammonia

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Journal of Energy Chemistry 2023年第12期87卷 408-415,I0011页

作者： Shuo Wang Yi Wang Yunfan Fu tianfu liu Guoxiong Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Energy University of Chinese Academy of SciencesBeijing 100039China

Hydrogen-bonded organic frameworks(HOFs),an emerging porous macrocyclic materials linked by hydrogen-bond,hold potential for gas separation and storage,sensors,optical,and ***,HOF-based electrocatalysts are rationally developed for nitrates reduction to ammonia,allowing not only to regulate wastewater pollution but also to accomplish carbon-neutral ammonia(NH_(3))*** preform high-throughput computational screening of thirty-six HOFs with various metals as active sites,denoted as HOF-M1,for nitrate reduction reaction(NO_(3)RR)toward NH_(3).We have implemented a hierarchical four-step screening strategy,and ultimately,HOF-Ti1 was selected based on its exceptional catalytic activity and selectivity in the NO_(3)RR *** additional analysis,we discovered that the d band center of the active metal sites serves as an effective parameter for designing and predicting the performance of HOFs in NO_(3)*** research not only showcases the immense potential of electrocatalysis in transforming NO_(3)RR into NH_(3)but also provides researchers with a compelling incentive to undertake further experimental investigations.

关键词： Nitrate reduction reaction Ammonia synthesis Hydrogen-bonded organic frameworks High-throughput calculations Electrocatalysts

Chelating Metal Ions in a Metal-Organic Framework for Constructing a Biomimetic Catalyst Through Post-modification

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Chemical Research in Chinese Universities 2022年第6期38卷 1542-1546页

作者： PANG Kuan XUE Huan liu Haixiong SUN Jing liu tianfu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002P.R.China School of Electronic Information and Electrical Engineering Shangluo UniversityShangluo726000P.R.China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China

Crystal engineering,as a burgeoning technology,has been widely used to construct metalloporphyrins biomimetic ***,a bimetallic metal-organic framework(MOF)was constructed by 4-(4-carboxyphenyl)-1,2,4-triazole ligand,Co2+and Zr4+metal ions by solvothermal reaction(named PFC-88).A N,N-chelation site was found between the two adjacent ligands in PFC-88,consequently a porphyrin-like structure was obtained through chelating Fe^(3+) in this site by post-modification,named *** result of a single crystal X-ray technology verified that Fe ions were successfully metalated in the N,N-chelation site of PFC-88,which is assisted by the X-ray absorption near-edge structure(XANES)*** o-phenylenediamine oxidation reaction was applied to assessing the catalytic activity of PFC-88-Fe,in which the absorbance increases of phenazine-2,3-diamine atλ=418 nm were recorded by absorption spectroscopy in kinetic mode,exhibiting the application potential as a biomimetic catalyst.

关键词： Metal-organic framework(MOF) Bimetallic MOF Crystal structure Metalation

Design and Synthesis of Bismuth-based Metal-Organic Frameworks for Photothermal Energy Conversion

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Chemical Research in Chinese Universities 2024年第6期40卷 964-969页

作者： WANG Rui WANG Ziyu YIN Qi liu Haixiong liu tianfu CAO Rong Department of Chemistry School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026P.R.China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350108P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

Template effect of the solvents plays a key role in metal-organic frameworks (MOFs) *** addition,Bi3+ has a flexible and changeable coordination configuration,which is conducive to the construction of structurally diverse ***,we demonstrate that these features can be integrated into two stable bismuth-based porphyrin MOFs (named PFC-100 and PFC-101) with a wide range of light *** studies demonstrate that PFC-101 with weaker interactions of adjacent porphyrin planes achieves 22.2% photothermal conversion efficiency (PTCE);1.5-fold higher than that of PFC-100 (14.3%) under 660 nm *** study may shed light on the impact of solvent templates on the synthesis of bismuth-based MOFs,not only enriching the MOFs library but also broadening the horizon of their potential applications.

关键词： Metal-organic frameworks(MOFs) Bismuth-based MOFs Design and synthesis Photothermal energy conversion

Plasmon-enhanced photocatalytic oxidative coupling of amines in the air using a delicate Ag nanowire@NH_(2)-UiO-66 core-shell nanostructures

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Chinese Chemical Letters 2024年第4期35卷 506-510页

作者： Yuan Zhang Shenghao Gong A.R.Mahammed Shaheer Rong Cao tianfu liu Fujian Science Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

MOF-based core-shell structures with high surface area, abundant active sites, and broad absorption bands are viable alternatives to traditional single-component photocatalysts. In this report, we describe the design and construction of delicate Ag nanowires@NH_(2)-UiO-66 with a core-shell structure for use as photocatalysts in imine synthesis under light. The optimized composites exhibited 80% imine production, which was higher than both MOF and Ag NWs. The significant improvement in photocatalytic activity under light may be attributed to the plasmonic effect of silver nanowires and their core-shell structure, which promotes the separation of electron-hole pairs. Moreover, the photocatalytic activity of the core-shell nanostructure may provide valuable insight into the design and construction of MOF-based composite photocatalysts for oxidative coupling of amines.

关键词： Metal-organic frameworks Plasmonic silver nanowires Photocatalyst Core-shell nanostructure Oxidative coupling of amines

Boosting electrocatalytic activity for CO_(2) reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus

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Journal of Energy Chemistry 2021年第3期30卷 143-150页

作者： Shuo Chen tianfu liu Samson O.Olanrele Zan Lian Chaowei Si Zhimin Chen Bo Li Key Laboratory of Functional Inorganic Material Chemistry(Ministry of Education of China) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina

Electrochemical reduction of CO_(2)(CERR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation,and carbon recycles *** metal catalysts suffered from low durability and sluggish kinetics impede the practical *** the other hand,doped carbon materials recently demonstrate superior catalytic performance in CERR,which shows the potential to diminish the problems of metal catalysts to some ***,we present the design and fabrication of nitrogen(N),phosphorus(P)co-doped metal-free carbon materials as an efficient and stable electrocatalyst for reduction of CO_(2) to CO,which exhibits an excellent performance with a high faradaic efficiency of 92%(-0.55 V ***)and up to 24 h stability.A series of characterizations including TEM and XPS verified that nitrogen and phosphorous are successfully incorporated into the carbon ***,the comparisons between co-doping and single doping catalysts reveal that co-doping can significantly increase CERR *** improved catalytic activity is attributed to the synergetic effects between nitrogen and phosphorous dopants,which effectively modulate properties of the active *** density functional theory(DFT)calculations were also performed to understand the synergy effects of *** is revealed that the phosphorous doping can significantly lower the Gibbs free energy of COOH^(*)***,the introduction of the second dopants phosphorous can reduce the reaction barrier along the reaction path and cause polarization of density of states at the Fermi *** changes can greatly enhance the activity of the *** a combined experimental and computational exploration,current work provides valuable insights into the reaction mechanism of CERR on N,P co-doped carbon catalysts,and the influence from synergy effects between dopants,which paves the way for the rational design of novel metal-free catalysts for CO2 electro-reduction.

关键词： Metal-free catalyst CO_(2)reduction Co-doping,DFT

The effects of local environment towards yield and selectivity on photocatalytic CO_(2)reduction catalyzed by metal-organic framework

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Chinese Chemical Letters 2023年第12期34卷 343-347页

作者： Qianqian Huang Rui Wang Xiya Li tianfu liu A.R.Mahammed Shaheer Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Fujian Science Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

The CO_(2)photoconversion is sensitive to the local reaction environment,of which activity and selectivity can be regulated by the change of reaction *** paper focuses on investigating the photocatalytic CO_(2)reduction behaviors of MOFs with the involvement of water under different reaction modes,including gas-solid and liquid-solid *** CO_(2)photoreduction in a liquid-solid system shows high performance in generating HCOOH with the selectivity of 100%.In contrast,the gas-solid system referring to the synergistic interaction of MOFs and H_(2)O vapor benefits to the formation of gas-phase products,such as CO and CH_(4).The possible mechanisms of photocatalytic CO_(2)reaction in two modes were investigated by in-situ Fourier-transform infrared spectroscopy,which indicates that the distinction in reaction consequence may result from the difference in CO_(2)chemisorbed modes and the proton *** choice of reaction system plays an important role in the achievement of high efficiency and selectivity for photocatalytic CO,reduction,whichis of great practical value in real-world applications.

关键词： Photocatalysis CO_(2) Reaction mode Yield Selectivity

In situ electrochemical reconstruction of Sr2Fe1.45Ir0.05Mo0.5O6-δ perovskite cathode for CO2 electrolysis in solid oxide electrolysis cells

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National Science Review 2023年第9期10卷 37-45页

作者： Yuxiang Shen tianfu liu Rongtan Li Houfu Lv Na Ta Xiaomin Zhang Yuefeng Song Qingxue liu Weicheng Feng Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences

Solid oxide electrolysis cells provide a practical solution for the direct conversion of CO2to other chemicals(***),however,an in-depth mechanistic understanding of the dynamic reconstruction of active sites for perovskite cathodes during CO2 electrolysis remains a great ***,we identify that iridium-doped Sr2Fe1.45Ir0.05Mo0.5O6-δ(SFIrM) perovskite displays a dynamic electrochemical reconstruction feature during CO 2 electrolysis with abundant exsolution of highly dispersed IrFe alloy nanoparticles on the SFIrM *** in situ reconstructed IrFe@SFIrM interfaces deliver a current density of 1.46 A cm-2while maintaining over 99% CO Faradaic efficiency,representing a 25.8%improvement compared with the Sr2Fe1.5Mo0.5O6-δ*** situ electrochemical spectroscopy measurements and density functional theory calculations suggest that the improved CO2electrolysis activity originates from the facilitated formation of carbonate intermediates at the IrFe@SFIrM *** work may open the possibility of using an in situ electrochemical poling method for CO2electrolysis in practice.

关键词： solid oxide electrolysis cell CO2 electrolysis, in situ electrochemical reconstruction metal/perovskite interface carbonate intermediates

Amorphous Sn(HPO_(4))_(2)-derived phosphorus-modified Sn/SnO_(x) core/shell catalyst for efficient CO_(2) electroreduction to formate

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Journal of Energy Chemistry 2023年第6期81卷 125-131,I0005页

作者： Chunfeng Cheng tianfu liu Yi Wang Pengfei Wei Jiaqi Sang Jiaqi Shao Yanpeng Song Yipeng Zang Dunfeng Gao Guoxiong Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great ***,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR *** total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V *** hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is ***,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 *** functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation.

关键词： CO_(2)electroreduction Structural evolution Reaction intermediate Phosphorus modification Stability

An inducible CO_2 concentrating mechanism in cyanobacterium Anabaena sp. strain PCC7120

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Chinese Science Bulletin 1999年第23期44卷 2177-2181页

作者： WU tianfu, SONG Lirong and liu YongdingInstitute of Hydrobiology , Chinese Academy of Sciences , Wuhan 430072 , China Corresponding author Institute of Hydrobiology Chinese Academy of Sciences Wuhan China

In order to define its characteristics of the photosynthetic utilization of CO2 and HCO3-when the ambient inorganic carbon changed, HCG (High-CO2-Growing Cells) of cyanobacteri-um Anabaena sp. strain PCC7120 were prepared. The growth rate of HCG was higher than that of LCG (low-CO2-growing cells, i.e. air-growing cells). When the HCG cells were transferred from 5% CO2 to air levels of CO2, a series of changes took place: its carbonic

关键词： HCG CCM photosynthetic affinity carboxysome.