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Rational design and synthesis of advanced metal-organic frameworks for electrocatalytic water splitting

Science China Chemistry 2023年第4期66卷 943-965页

作者： Yu-Jia Tang ya-qian lan School of Chemistry and Materials Science Institute of Advanced Materials and Flexible Electronics(IAMFE)Nanjing University of Information Science and TechnologyNanjing 210044China School of Chemistry South China Normal UniversityGuangzhou 510006China

As a promising and significant technology for hydrogen production,electrocatalytic water splitting is a research hotspot in the energy conversion field for alleviating the global energy crisis and achieving carbon neutrality ***-organic frameworks(MOFs)have been widely investigated as catalyst candidates with remarkable activity and long-term electrocatalysis durability owing to their precise and tailorable structures:tunable pore channels in the range of micropore/mesopore promote the mass/electron transfer;high specific surface areas expose abundant active species;modified metal nodes can serve as active sites;versatile organic ligands can be functionalized to further enhance the electrocatalytic *** this review,recent advances in the rational design and synthesis of advanced MOF electrocatalysts for water splitting are presented in the following ***,we analyze the design concepts of MOF electrocatalysts from the perspective of their distinct and modifiable ***,three common synthesis techniques of MOF electrocatalysts are briefly ***,we focus on the classification of different MOFs for robust electrocatalytic water splitting,including pristine MOFs,mixed-metallic MOFs,MOF nanosheets,electrically conductive MOFs,MOFs on substrates,and polyoxometalate-based ***,summary and outlook are proposed to uncover the next generation of advanced MOFs for electrochemical energy conversion applications.

关键词： metal-organic frameworks water splitting electrocatalysis hydrogen evolution reaction oxygen evolution reaction polyoxometalates

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Boosting CO_(2) electroreduction performance over fullerene-modified MOF-545-Co promoted by π –π interaction

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Chinese Chemical Letters 2023年第4期34卷 559-563页

作者： Xue Dong Zhifeng Xin Dong He Jia-Ling Zhang ya-qian lan qian-Feng Zhang Yifa Chen Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa’anshan 243002China National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Key Lab.of ETESPG(GHEI)School of ChemistrySouth China Normal UniversityGuangzhou 510006China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread applications. Herein, fullerene molecules(i.e., C60and C70) have been successfully introduced into the pore-channels of a Co-porphyrin based MOF through a facile strategy. Thus-obtained hybrid materials present higher electron-transfer ability, enhanced CO_(2)adsorption-enthalpy and CO_(2)electroreduction activity. Notably, the charge transfer resistance(Rct) of C60@MOF-545-Co is almost 5 times lower of than that of MOF-545-Co, as well as 1.5 times increased for the CO_(2)adsorption enthalpy. As expect, the FECO of C60@MOF-545-Co(97.0%) is largely higher than MOF-545-Co(70.2%), C60@MOF-545(19.4%), C60(11.5%)and physical mixture(70.3%) and presented as one of the best CO_(2)electroreduction catalysts reported in H-cell system. The facile strategy would give rise to new insight into the exploration of powerful MOFbased hybrid materials in high-efficiency CO_(2)electroreduction.

关键词： Fullerene Metal organic framework Electrocatalytic performance π-πinteraction CO_(2)RR

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Two new pseudo-isomeric nickel(Ⅱ)metal-organic frameworks with efficient electrocatalytic activity toward methanol oxidation

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Rare Metals 2021年第2期40卷 489-498页

作者： Shan Liu Xiao Wang Hong-Guang Yu ya-Pan Wu Bo Li ya-qian lan Tao Wu Jian Zhang Dong-Sheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang443002China

Searching for non-noble metal catalysts with high activities and low price is critical to the commercialization of methanol oxidation in the process of fuel ***,two new pseudo-isomeric Ni metal-organic frameworks(Ni-MOFs)(CTGU-17/CTGU-18)have been prepared with 1,4-naphthalenedi-carboxylate(H_(2)NDC),4,4’-dipyridyl amine(DPA)and Ni(ClO_(4))_(2)under hydrothermal *** phase contains one water molecule,but differs dramatically in its bonding to the framework,resulting in different topological networks with fourfold interpenetrating 4-connected dia net(CTGU-17)and(3,7)-connected net(CTGU-18)and diverse electrocatalytic performance for methanol oxidation reaction(MOR).Remarkably,by combining each MOF with the conductive additive,acetylene black(AB),a composite material,AB&CTGU-18(2:4)was confirmed to have an excellent performance for MOR with a high mass specific peak current of 442.3 mA·mg^(-1).The enhanced electrocatalytic activities and robustness might be attributed to the synergetic effect of acetylene black and the active metal centers of MOFs particles for methanol *** present work would provide a new insight for the rational design of MOFs-based composites with enhanced methanol oxidation reaction performance.

关键词： Nickel(Ⅱ) MOFs Composite materials Electrocatalysis Methanol oxidation

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Cu cluster embedded porous nanofibers for high-performance CO_(2) electroreduction

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Chinese Chemical Letters 2023年第4期34卷 542-546页

作者： Zhifeng Xin Zibo Yuan Jingjing Liu Xinjian Wang Kejing Shen Yifa Chen ya-qian lan Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa’anshan 243002China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Metal-doped carbon materials, as one of the most important electrocatalytic catalysts for CO_(2)reduction reaction(CO_(2)RR), have attracted increasing attention. Herein, a series of Cu cluster embedded highly porous nanofibers have been prepared through the carbonization of electro-spun MOF/PAN *** obtained Cu cluster doped porous nanofibers possessed fibrous morphology, high porosity, conductivity, and uniformly dispersed Cu clusters, which could be applied as promising CO_(2)RR catalysts. Specifically, best of them, MCP-500 exhibited high catalytic performance for CO_(2)RR, in which the Faradaic efficiency of CO(FECO) was as high as 98% at-0.8 V and maintained above 95% after 10 h continuous electrocatalysis. The high performance might be attributed to the synergistic effect of tremendously layered graphene skeleton and uniformly dispersed Cu clusters that could largely promote the electron conductivity, mass transfer and catalytic activity during the electrocatalytic CO_(2)RR process. This attempt will provide a new idea to design highly active CO_(2)RR electrocatalyst.

关键词： Electrocatalysis Cu cluster Porous nanofiber Electrospinning CO_(2)RR

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Evolution exploration and structure prediction of Keggin-type group IVB metal-oxo clusters

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Chinese Chemical Letters 2024年第5期35卷 487-492页

作者： Run-Han Li Tian-Yi Dang Wei Guan Jiang Liu ya-qian lan Zhong-Min Su School of Chemistry South China Normal UniversityGuangzhou 510006China Institute of Functional Material Chemistry Faculty of ChemistryNortheast Normal UniversityChangchun 130024China Institute of Theoretical Chemistry Jilin UniversityChangchun 130023China

The fascinating chemical structure and broad application prospect of Keggin-type polyoxometalates(POMs)have attracted many chemists to explore and discover *** the traditional Keggin,larger metal atomic radius,higher metal coordinated numbers,lower metal valence states and other features allow the group IVB metal-based Keggin(IVB-Keggin)more space and unknown in terms of structure and ***,density functional theory(DFT)calculations were performed to explore the influences including cores,shells,caps,and terminal ligands,et *** IVB-Keggin,and analyze the possibility of novel structure *** the perspective of multi-layer onion-like clusters,molecular energy level,host-guest interaction energy,surface charge and covalent bond polarity can be further adjusted to achieve the oriented design of functional *** insights are expected to provide theoretical support for experimental synthesis,opening a new perspective to understand the growth of Keggin.

关键词： Keggin Metal-oxo clusters Group IVB Onion pattern DFT

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Identification of the activity source of CO2 electroreduction by strategic catalytic site distribution in stable supramolecular structure system

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National Science Review 2021年第3期8卷 78-87页

作者： Sheng-Nan Sun Ning Li Jiang Liu Wen-Xin Ji Long-Zhang Dong Yi-Rong Wang ya-qian lan Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials Science Nanjing Normal University School of Chemistry and Chemical Engineering Yangzhou University State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering Ningxia University

Identification of the real catalytic site in CO;2;reduction reaction（CO;2;RR） is critical for the rational design of catalysts and the understanding of reactive *** this study,the catalytic activity of pyridine-containing materials was for the first time structurally demonstrated in CO;2;RR by crystalline supramolecular coordination compounds model *** system consists of three stable supramolecular coordination compounds（Ni-TPYP,Ni-TPYP-1 and Ni-TPP） with different numbers（4,2 and 0） of active pyridine groups（*** pyridine nitrogen atoms）.The electrocatalytic test results show that with the decrease of the number of active pyridine groups,the CO;2;RR performance is gradually reduced,mainly showing the reduction of highest FE;CO;（99.8%,83.7% and 25.6%,respectively）.The crystallographic,experimental and theoretical evidences prove that the CO;2;RR activity is more likely derived from uncoordinated pyridine nitrogen than the electrocatalytic inert metal nickel in porphyrin *** work serves as an important case study for the identification of electrocatalytic activity of pyridine-containing materials in CO;2;RR by simple supramolecular model system.

关键词： strategic catalytic site distribution supramolecular structure system active source CO2 electroreduction

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Selective photosynthesis of Z-olefins through crystalline metal-organic cage-initiated expeditious cascade reactions

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Carbon Energy 2024年第3期6卷 118-131页

作者： Jia-Ni Lu Yunze Huang Yuan-Sheng Xia Long-Zhang Dong Lei Zhang Jing-Jing Liu lan-Gui Xie Jiang Liu ya-qian lan Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina School of Chemistry South China Normal UniversityGuangzhouChina

The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical ***,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial ***,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton *** the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen *** them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple ***“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions.

关键词： alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins

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Large eddy simulation of unsteady flow in gas-liquid separator applied in thorium molten salt reactor

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Nuclear Science and Techniques 2018年第5期29卷 10-18页

作者： Jing-Jing Li ya-lan qian Jun-Lian Yin Hua Li Wei Liu De-Zhong Wang School of Mechanical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Shanghai Institute of Applied Physics Shanghai 201800China

Axial gas-liquid separators have been adopted in fission gas removal systems for the development of thorium molten salt reactors. In our previous study, we observed an unsteady flow phenomenon in which the flow pattern is directly dependent on the backpressure in a gas-liquid separator; however, the underlying flow mechanism is still unknown. In order to move a step further in clarifying how the flow pattern evolves with a variation in backpressure, a large eddy simulation(LES) was adopted to study the flow field evolution. In the simulation, an artificial boundary was applied at the separator outlet under the assumption that the backpressure increases linearly. The numerical results indicate that the unsteady flow feature is captured by the LES approach, and the flow transition is mainly due to the axial velocity profile redistribution induced by the backpressure variation. With the increase in backpressure,the axial velocity near the downstream orifice transits from negative to positive. This change in the axial velocity sign forces the unstable spiral vortex to become a stable rectilinear vortex.

关键词： Swirl flow Thorium molten salt reactor Computational fluid dynamics Large eddy simulation

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Crystalline porous materials for catalytic conversion of lignin-related substances

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Aggregate 2024年第3期5卷 142-163页

作者： Qing Huang Pengfei Wu Xiu-Fen Li Yi-Rong Wang Dan Tian ya-qian lan College of Materials Science and Engineering Nanjing Forestry UniversityNanjingJiangsuP.R.China School of Chemistry South China Normal UniversityGuangzhouP.R.China Co-Innovation Center for Sustainable Forestry in Southern China Nanjing Forestry UniversityNanjingJiangsuP.R.China

The conversion of the biomass into eco-friendly fuels and chemicals has been exten-sively recognized as the essential pathway to achieve the sustainable economy and carbon neutral ***,as a kind of promising biomass energy,has been certiﬁed to produce the high-valued chemicals and *** efforts have been made to develop various catalysts for lignin catalytic *** metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)belong to very important heterogeneous porous catalysts due to their regular porous struc-tures,high speciﬁc surface area,and precisely tailored *** the review,theﬁrst part focused on the catalytic conversion of lignin,lignin model compounds,and lignin derivatives using the pristine MOFs,functional MOF composites,and MOF-derived *** second part summarized the catalytic conversion of lignin model compounds using pristine COFs and functional COF *** review here mainly concentrated on the design of the materials,screening of catalytic conditions,and explorations of the corresponded ***ﬁcally,(1)we summarized the MOF-and COF-based materials for the effects on the catalytic trans-formation of lignin-related substances;(2)we emphasized the catalytic mechanism of C–C and C–O bonds cleavage together with the structure–activity relationships;(3)we in-depth realized the relationship between the chemical/electronic/structural properties of the MOF-and COF-based catalysts and their catalytic performance for lignin-related ***,the challenges and future perspectives were also discussed on the catalytic conversion of lignin-related substances by MOF-and COF-based catalysts.

关键词： catalytic conversion covalent organic frameworks lignin lignin derivatives lignin model compounds metal-organic frameworks

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MOF-Derived Materials Enabled Lithiophilic 3D Hosts for Lithium Metal Anode—A Review

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Chinese Journal of Chemistry 2023年第15期41卷 1861-1874页

作者： Tao Wei Jiahao Lu Mengting Wang Cheng Sun Qi Zhang Sijia Wang yanyan Zhou Daifen Chen ya-qian lan School of Energy and Power Jiangsu University of Science and TechnologyZhenjiangJiangsu 212003China School of Chemistry South China Normal University55 West Zhongsan Rd.GuangzhouGuangdong 510006China

Comprehensive Summary This work systematically reviews recent progresses in the applications of MOF-derived materials modified 3D porous conductive framework as hosts for uniform lithium deposition in LMBs.A series of commonly used lithiophilic materials and several kinds of representative MOF-derivation-modified 3D hosts as lithium metal anode(LMA)are ***,the challenges and future development of employing MOF-derived materials to modify the 3D porous conductive framework for LMA are included.

关键词： Metal-organic frameworks(MOFs) Lithium metal anode(LMA) Lithiophilic materials Three-dimensional(3D)host MOF-derived materials Interfacial modification Lithium-metal batteries Electrochemistry

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