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CCS Chemistry 2024年第8期6卷 1978-1986页

作者： Cheng-Peng Liang Jia-Run Huang Hao-Lin Zhu Zhen-Hua Zhao Can Yu pei-qin liao Xiao-Ming Chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular EngineeringSchool of ChemistrySun Yat-sen UniversityGuangzhouGuangdong 510275 Institute of High Energy Physics Chinese Academy of Sciences(CAS)Beijing 100049

Precise regulation of the coordination environment of a metal active center is very important but remains a ***,single-atom Ni catalysts with a combined N-and C-coordination structure(Ni-NC_(3))and N-coordination structure(Ni-N4)were prepared by modulating the side groups of organic ligands in the corresponding precursor metal–azolate *** with the Ni-N4 site,the d-band center of 3d orbitals of the Ni atom in Ni-NC_(3)was more significantly shifted to the Fermi energy level;thus,the Ni-NC_(3)catalytic site was superior to activating CO_(2)molecule into the*COOH *** a result,Ni-NC_(3)exhibited an exceptionally high performance for CO_(2)-to-CO conversion with a Faradaic efficiency of 98.4%,an energy efficiency of>50%,as well as an industrial current density of∼300 mA cm^(−2) in neutral *** high performance could be retained for at least 70 *** work reveals the importance of modulating the coordination environment in the electrochemical CO_(2)reduction reaction and provides a possible way to rational design of electrocatalysts for highly efficient conversion of CO_(2)to target products.

关键词： single-atom Ni catalysts first coordination shell porous nitrogen-doped carbon electrochemical CO_(2)reduction reaction coordination environment

一例整合了三联吡啶钌和卟啉锌的金属-有机框架材料用于光催化二氧化碳还原全反应

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物理化学学报 2024年第4期40卷 4-10页

作者：陈慧滢朱浩林廖培钦陈小明中山大学化学学院生物无机与合成化学教育部重点实验室广州510275

利用源源不断的太阳能,将CO_(2)和水转化为增值化学品,是缓解温室效应与能源危机的一种有前途的方法。由于催化体系中的不同功能性部分难以实现氧化与还原反应的耦合,使用水作为还原剂实现光催化CO_(2)还原是一项具有挑战性的工作。金... 详细信息

利用源源不断的太阳能,将CO_(2)和水转化为增值化学品,是缓解温室效应与能源危机的一种有前途的方法。由于催化体系中的不同功能性部分难以实现氧化与还原反应的耦合,使用水作为还原剂实现光催化CO_(2)还原是一项具有挑战性的工作。金属有机框架(metal-organic framework,MOF)由于其较大的比表面积、多样化的活性位点和结构可调性,是CO_(2)光催化还原全反应的良好备选材料。本文中,我们首先整合了具有光活性的锌(Ⅱ)卟啉基元与联吡啶钌(Ⅱ)基元,构建了一种MOF光催化剂,记作PCN-224(Zn)-Bpy(Ru)。为了进行比较,还合成了两种仅具有锌(Ⅱ)卟啉或联吡啶钌(Ⅱ)基元的同构MOF,分别记作PCN-224(Zn)-Bpy和PCN-224-Bpy(Ru)。由测试结果可知,PCN-224(Zn)-Bpy(Ru)在乙腈和水混合溶液中表现出对CO_(2)还原可观的光催化活性(CO产率为7.6μmol·g^(-1)·h^(-1)),无需额外添加助催化剂、光敏剂或牺牲剂。通过质谱仪观测到^(13)CO(m/z=29)、^(13)C^(18)O(m/z=31)、^(16)O^(18)O(m/z=34)和^(18)O_(2)(m/z=36)信号,表明CO_(2)和H_(2)O分别作为CO和O_(2)的碳源和氧源,这进一步证实了光催化CO_(2)还原与H_(2)O氧化的耦合。然而,在相同条件下对PCN-224-Bpy(Ru)与PCN-224(Zn)-Bpy的光催化性能进行测试,CO产率分别仅为1.5与0μmol·g^(-1)·h^(-1)。机理研究表明,PCN-224(Zn)-Bpy(Ru)的最低未占据分子轨道(LUMO)电位比CO_(2)/CO的氧化还原电位更负,而最高占据分子轨道(HOMO)电位比H_(2)O/O_(2)的氧化还原电位更正,在热力学上满足了光催化CO_(2)还原全反应的要求。相比之下,不含联吡啶钌(Ⅱ)基元的PCN-224(Zn)-Bpy的HOMO电位更负于H_(2)O/O_(2)的氧化还原电位,这表明联吡啶钌(Ⅱ)基元在热力学上是光催化CO_(2)还原全反应所必需的。此外,光致发光光谱中,荧光几乎被PCN-224(Zn)-Bpy(Ru)猝灭,且平均光致发光寿命比PCN-224(Zn)-Bpy和PCN-224-Bpy(Ru)更长,这表明PCN-224中光生载流子的复合率较低。与PCN-224(Zn)-Bpy和PCN-224-Bpy(Ru)相比,PCN-224的光电流更高,这一现象也支持了中后者光生载流子的复合率较低这一结论。总而言之,在光催化CO_(2)还原过程中,锌卟啉(Ⅱ)配体既作为光敏单元,又作为CO_(2)还原活性位点,而联吡啶钌(Ⅱ)基元与锌(Ⅱ)卟啉基元的结合可以优化光催化剂的能带结构,进而促进光催化CO_(2)还原与H_(2)O氧化的耦合,从而实现了高效光催化CO_(2)还原全反应。

关键词：金属有机框架锌(Ⅱ)卟啉衍生物联吡啶(Ⅱ)钌配合物光生电荷光催化CO_(2)还原

设计双功能电催化剂以提高电化学二氧化碳还原反应的电解池能量效率

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中国科学：化学 2024年第9期54卷 1516-1521页

作者：黄嘉润张梦迪廖培钦陈小明中山大学生物无机与合成化学教育部重点实验室中山大学化学学院广州510275 化学与精细化工广东省实验室汕头515021

电化学二氧化碳还原反应(eCO_(2)RR)因其在实现碳中和方面的巨大潜力而受到广泛关注,目前科研人员也致力于开发高效的eCO_(2)RR催化剂.然而,作为电解池关键组成部分的阳极反应却常常被忽视.电解池的能量效率和催化产物的价值在很大程度... 详细信息

电化学二氧化碳还原反应(eCO_(2)RR)因其在实现碳中和方面的巨大潜力而受到广泛关注,目前科研人员也致力于开发高效的eCO_(2)RR催化剂.然而,作为电解池关键组成部分的阳极反应却常常被忽视.电解池的能量效率和催化产物的价值在很大程度上取决于阴极和阳极的总槽电压.遗憾的是,大多数关于eCO_(2)RR和阳极反应双功能催化剂的研究报告显示,其电流密度普遍较低,远未达到商业应用的要求.近年来,在催化剂中整合氧化和还原位点的策略被证明是提高eCO_(2)RR电解池的总能量效率的可行方法.本文基于这种策略的部分代表性研究进行了阐述,并探讨了未来研究的潜在机遇.

关键词：电催化二氧化碳还原电催化剂碳中和双功能电催化剂能量效率

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Controlling flexibility of metal–organic frameworks

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National Science Review 2018年第6期5卷 907-919页

作者： Jie-Peng Zhang Hao-Long Zhou Dong-Dong Zhou pei-qin liao Xiao-Ming Chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen University Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou University

Framework flexibility is one of the most important characteristics of metal–organic frameworks(MOFs),which is not only interesting, but also useful for a variety of applications. Designing, tailoring or controlling framework flexibility of MOFs is much more difficult than for static structural features such as the framework topology and pore size/shape. Nevertheless, with in-depth understanding of the relationship between framework flexibility and the host framework structure, guest loading and other aspects such as the crystal size/morphology and external physical environment, some strategies have been developed for controlling the flexibility of MOFs and the corresponding properties, which are summarized and discussed in this review.

关键词： porous coordination polymers metal–organic frameworks flexibility dynamism adsorption structural transformation

A novel pillared-layer-type porous coordination polymer featuring three-dimensional pore system and high methane storage capacity

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Science China Chemistry 2016年第8期59卷 970-974页

作者： Jiao-Min Lin Chun-Ting He pei-qin liao Dong-Dong Zhou Jie-Peng Zhang Xiao-Ming Chen Key Laboratory of Bioinorganic and Synthetic Chemistry Ministry of EducationSchool of Chemistry and Chemical Engineering Sun Yat-Sen University Guangzhou 510275 China

Solvothermal reaction of Zn（NO3）2, 4-（1H-pyrazol-4-yl）pyridine （Hpypz） and 1,3,5-benzenetricarboxylic acid （H3btc） in N,N-dimethylacetamide （DMA） produced a new porous coordination polymer [Zns（pypz）4（btc）2] （1）. Single-crystal X-ray diffraction study of 1 showed that deprotonated pypz^- ligands served as 1,2,4-triazolate-like ligands, linking Zn（II） ^＋ ions to form porous two-dimensional （2-D） sql-a layers {Zn（pypz）} , which were further connected by eight-legged pillars {Zn2（btc）4（H2O）2}8- based on the typical paddlewheel dinuclear Zn2（RCOO）4（H20）2 cluster to form a novel type of non-interpenetrated pillared-layer framework with 3-D intersecting pore system and large pore volume. Gas sorption measurements revealed that 1 possesses large BET surface area of 2061 m^2g^-1 and very high methane total uptake of 245 cm^3（STP） cm^-3 at 298 K and 65 bar.

关键词： metal-organic framework network topology eight-legged pillar methane storage

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A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO_(2)to C_(2+)Products

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Chemical Research in Chinese Universities 2024年第4期40卷 664-669页

作者： LIU Yuan-Yuan ZHU Hao-Lin liao pei-qin CHEN Xiao-Ming Key Laboratory of Bioinorganic and Synthetic Chemistry Ministry of EducationGBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou510275P.R.China Chemistry and Chemical Engineering Guangdong Laboratory Shantou515031P.R.China

Driven by renewable or excess electrical energy,electrochemical CO_(2)reduction reaction(eCO_(2)RR)represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO_(2)and H_(2)O.C_(2+)products are one of the most economically valuable products among the reduction species of eCO_(2)RR,but there are still some challenges,such as low selectivity or low current *** this work,we showed that a copper-based metal-azolate framework(MAF),denoted as MAF-203,exhibits the high performance of eCO_(2)RR to yield C_(2+)products with the Faradaic efficiency(C_(2+))of 52.5%and a current density of 660 mA/cm^(2)at-1.2 V *** in a flow cell device under alkaline *** experiment,in situ infrared spectroscopy and the density functional theory(DFT)calculations showed that the electron donating effect of methyl substituents on organic ligands of the copper-based MAF could enhance the ligand field and activation of key intermediates(*CO and*CHO species),thus promoting the coupling of*CO and*CHO for yielding C_(2+)products.

关键词： Metal-organic framework Carbon dioxide Electroreduction C_(2+)product Metal-azolate framework

Parallelization strategies for resolved simulations of fluid-structure-particle interactions

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Applied Mathematics and Mechanics(English Edition) 2024年第5期45卷 857-872页

作者： Jianhua qin Fei liao Guodan DONG Xiaolei YANG The State Key Laboratory of Nonlinear Mechanics Institute of MechanicsChinese Academy of SciencesBeijing 100190China Interdisciplinary Center for Fundamental and Frontier Sciences Nanjing University of Science and TechnologyJiangyin 214443Jiangsu ProvinceChina School of Aeronautics Northwestern Polytechnical UniversityXi'an 710072China School of Engineering Sciences University of Chinese Academy of SciencesBeijing 100049China

Fluid-structure-particle interactions in three spatial dimensions happen in many environmental and engineering *** paper presents the parallel algorithms for the hybrid diffuse and sharp interface immersed boundary(IB)method developed in our previous *** the moving structure modeled using the sharp interface IB method,a recursive box method is developed for efficiently classifying the background grid *** the particles modeled using the diffuse interface IB method,a‘master-slave’approach is *** the particle-particle interaction(PPI)and particle-structure interaction(PSI),a fast algorithm for classifying the active and inactive Lagrangian points,which discretize the particle surface,is developed for the‘dry’contact *** results show that the proposed recursive box method can reduce the classifying time from 52seconds to 0.3 *** parallel efficiency is obtained for cases with different particle ***,the lubrication model is utilized when a particle approaches a wall,enabling an accurate simulation of the rebounding phenomena in the benchmark particle-wall collision *** last,the capability of the proposed computational framework is demonstrated by simulating particle-laden turbulent channel flows with rough walls.

关键词： particle-resolved direct numerical simulation particle-laden flow complex geometry resolved fluid-structure-particle interaction(RFSPI) immersed boundary(IB)method

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Local Weak Hydrogen Bonds Significantly Enhance CO_(2)Electroreduction Performances of a Metal-Organic Framework

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CCS Chemistry 2023年第1期5卷 145-151页

作者： Yu Wang Ning-Yu Huang Hao-Yu Wang Xue-Wen Zhang Jia-Run Huang pei-qin liao Xiao-Ming Chen Jie-Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275

Technological application of the electrochemical reduction of CO_(2)relies on efficient *** demonstrate that the introduction of amino groups alongside the porphyrin cobalt centers in a metal-organic framework(MOF)can dramatically accelerate the electrochemical CO_(2)reduction performance.A classic cobalt porphyrin-based MOF showing moderate CO_(2)-to-CO electroreduction performance(turnover frequency[TOF]=0.20 s^(−1),Faradic efficiency[FE]=47.4%)is *** molecular design of the porphyrin-based ligand,amino groups are introduced alongside the cobalt center,giving remarkably enhanced CO_(2)-to-CO electroreduction performance as high as FE 99.4%,current density 7.2 mA cm^(−2),and TOF 21.17 s^(−1),in a nearneutral aqueous solution at a low overpotential of 525 *** functional theory calculations showed that the prepositioned amino groups,although located not sufficiently close to the active center,serve as hydrogen-bonding donors to stabilize the intermediate Co-CO_(2)adduct and impede the formation of Co-H_(2)O adduct,which not only promotes the CO_(2)reduction reaction but also restrains the hydrogen evolution reaction.

关键词： CO_(2)electroreduction metal-organic frameworks hydrogen bond porphyrin amino groups

Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei qin Rui Wang Zilong Yuan pei Xiao Deli Wang Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper t... 详细信息

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

Kaempferol ameliorated levodopa-induced dyskinesia in experimental rats: A role of brain monoamines, cFOS, FosB, Parkin, Pdyn, TH, and p-JNK

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BIOCELL 2024年第3期48卷 513-523页

作者： pei qin MIAO LIU XIN WANG JIANHUA MA Geriatrics Department Chengde Central HospitalChengde067000China

Background:L-dopa(Levodopa)is well known for managing PD(Parkinson’s disease);however,its prolonged use caused dyskinesia(LID).Due to the varied presentation of LID,effective treatment options are *** reported their neuroprotective activity by ameliorating acetylcholinesterase,monoamine oxidase,and neuroinﬂ*** is anotherﬂavonoid bearing these ***:To evaluate neuroprotective activity of kaempferol in dyskinetic ***:PD was developed in Sprague-Dawley rats by injecting combination of L-ascorbic acid(10µL)+6-OHDA(12µg)in medial forebrain bundle to induce neuronal damage in substantial nigra(SNr).LID was induced by administrating combination of L-dopa(20 mg/kg)+benserazide HCl(5 mg/kg)for 42 *** were concomitantly treated with amantadine(40 mg/kg)or kaempferol(25,50,and 100 mg/kg,p.o.).Results:Kaempferol(50 and 100 mg/kg)markedly(p<0.05)inhibited LID-induced abnormal involuntary movements(AIMs)and alternation in motor *** administration considerably(p<0.05)inhibited reduced mitochondrial complex activities,serotonin and dopamine levels,Bcl-2,and Tyrosine hydroxylase protein expressions in ***,kaempferol considerably(p<0.05)attenuated increased cFOS,FosB,Parkin,and Pdyn mRNAs expressions,Bax,cleaved caspase-3,caspase-3,and pJNK proteins levels;DOPAC and 5-HIAA levels in SNr.A positive correlation was reported between cFOS,FosB,Parkin,Pdyn,apoptosis,and TH with ***:Kaempferol effectively attenuated L-dopa-induced AIMs and dyskinesia via amelioration of alterations in cFOS,FosB,Parkin,Pdyn,Tyrosine hydroxylase,and apoptosis in the brain SNr.

关键词： AIMs cFOS Kaempferol Levodopa-induced dyskinesia Pdyn