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Metal-organic frameworks derived transition metal phosphides for electrocatalytic water splitting

Journal of Energy Chemistry 2022年第5期31卷 494-520页

作者： Li-Ming Cao Jia Zhang Li-Wen Ding Zi-Yi Du chun-ting he Key Laboratory of Functional Small Molecules for Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022JiangxiChina Key Laboratory for Green Chemistry of Jiangxi Province Nanchang 330022JiangxiChina

It is critical to synthesize high-efficiency electrocatalysts to boost the performance of water splitting to meet the requirements of industrial applications. Metal-organic frameworks(MOFs) can function as ideal molecular platforms for the design of highly reactive transition metal phosphides(TMPs), a kind of candidates for high-efficiently electrocatalytic water splitting. The intrinsic activity of the electrocatalysts can be greatly improved via modulating the electronic structure of the catalytic center through the MOF precursors/templates. Moreover, the carbon layer converted in-situ by the organic ligands can not only protect the TMPs from being degraded in the harsh electrochemical environments, but also avoid agglomeration of the catalysts, thereby promoting their activities and stabilities. Furthermore,heteroatom-containing ligands can incorporate N, S or P, etc. atoms into the carbon matrixes after conversion, regulating the coordination microenvironments of the active centers as well as their electronic structures. In this review, we first summarized the latest developments in MOF-derived TMPs by the unique advantages in metal, organic ligand, and morphology regulations for electrocatalytic water splitting. Secondly, we concluded the critical scientific issues currently facing for designing state-of-the-art TMP-based electrocatalysts. Finally, we presented an outlook on this research area, encompassing electrocatalyst construction, catalytic mechanism research, etc.

关键词： Metal-organic framework Transition metal phosphide Water splitting Electrocatalyst Electronic structure

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Atomically Dispersed Dual‑Metal Sites Showing Unique Reactivity and Dynamism for Electrocatalysis

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Nano-Micro Letters 2023年第8期15卷 192-204页

作者： Jun‑Xi Wu Wen‑Xing Chen chun‑ting he Kai Zheng Lin‑Ling Zhuo Zhen‑Hua Zhao Jie‑Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275People’s Republic of China Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022People’s Republic of China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China

The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional ***,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed *** of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water *** importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH *** functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.

关键词： Metal-organic frameworks Atomically dispersed catalyst Hydrogen bond Overall water splitting

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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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Thermal-induced reversible ferroelastic phase transition in a new bromethyl-substituted molecular rotor

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Science China Chemistry 2015年第7期58卷 1137-1143页

作者： Bao-Ying Wang chun-ting he Bo Huang Wei-Jian Xu Wei Xue Zi-Yi Du Wei-Xiong Zhang Xiao-Ming Chen Key Laboratory of Bioinorganic and Synthetic Chemistry Ministry of Education School of Chemistry & Chemical Engineering Sun Yat-Sen University College of Chemistry & Chemical Engineering Gannan Normal University

A new bromethyl-substituted molecular rotor, [Cu（dabcoCH2Br）（H2O）Br3] （dabcoCH2Br＋=1-（2-bromethyl）-1,4-diazoniabi- cyclo[2.2.2]octane cation）, which belongs to a family of balomethyl-substituted molecular rotors, was synthesized and struc- turally characterized. The reversible phase transition at ca. 250 K was well established for this molecular rotor by thermal analyses, variable-temperature X-ray diffraction, and variable temperature dielectric measurements. The order-disorder trans- formation of the rotator part （dabco moiety） causes ferroelastic phase transition with an Aizu notation of mmmF2/m from high- temperature orthorhombic phase （Pbnm） to low-temperature monoclinic phase （P21/n）. More important, in reference to the density functional theory calculations and structural analyses, the key factors to tune the phase transition behaviors were dis- cussed in detail for this family of halomethyl-substituted molecular rotors.

关键词： ferroelastic phase transition molecular rotor confined space

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Flexibility of Metal-Organic Framework Tunable by Crystal Size at the Micrometer to Submillimeter Scale for Efficient Xylene Isomer Separation

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Research 2019年第1期2019卷 433-441页

作者： Xiao Yang Hao-Long Zhou chun-ting he Zong-Wen Mo Jia-Wen Ye Xiao-Ming Chen Jie-Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Understanding,controlling,and utilizing the flexibility of adsorbents are of great importance and *** with conventional solid materials,downsizing to the nanoscale is emerging as a possible strategy for controlling the flexibility of porous coordination polymers(or metal-organic frameworks).We report a unique flexibility controllable by crystal size at the micrometer to submillimeter *** removal transforms[Cu_(2)(pypz)_(2)]·0.5p-xylene(MAF-36,Hpypz=4-(1H-pyrazol-4-yl)pyridine)with one-dimensional channels toα-[Cu_(2)(pypz)_(2)]with discrete small cavities,and further heating gives a nonporous isomerβ-[Cu_(2)(pypz)_(2)].Both isomers can adsorb p-xylene to give[Cu_(2)(pypz)_(2)]·0.5p-xylene,meaning the coexistence of guest-driven flexibility and shape-memory *** phase transition temperature fromα-[Cu_(2)(pypz)_(2)]toβ-[Cu_(2)(pypz)_(2)]decreased from~270℃ to~150℃ by increasing the crystal size from the micrometer to the submillimeter scale,ca.2-3 orders larger than those of other size-dependent ***-crystal X-ray diffraction showed coordination bond reconstitution and chirality inversion mechanisms for the phase transition,which provides a sufficiently high energy barrier to stabilize the metastable phase without the need of downsizing to the *** virtue of the crystalline molecular imprinting and gate-opening effects,α-[Cu_(2)(pypz)_(2)]andβ-[Cu_(2)(pypz)_(2)]show unprecedentedly high p-xylene selectivities of 16 and 51,respectively,as well as ultrafast adsorption kinetics(<2 minutes),for xylene isomers.

关键词： isomers coordination adsorbent

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Non-3d metal modulated zinc imidazolate frameworks for CO_(2) cycloaddition in simulated flue gas under ambient condition

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Chinese Chemical Letters 2023年第7期34卷 390-393页

作者： Yan-Tong Xu Zi-Ming Ye De-Xuan Liu Xiao-Yun Tian Dong-Dong Zhou chun-ting he Xiao-Ming Chen MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640China MOE Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China

Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO_(2) are still required for the ***, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO_(4)^(2–)or WO_(4)^(2–)units, which can catalyse cycloaddition of CO_(2) and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO_(2) and 98% yield after 48 h in simulated flue gas(15% CO_(2)+ 85% N_(2)),respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO_(4)^(2–)unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.

关键词： Non-3d metal modulation Metal-organic framework CO_(2)fixation Flue gas Cycloaddition reaction

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Mild metal-organic-gel route for synthesis of stable sub-5-nm metal-organic framework nanocrystals

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Nano Research 2017年第11期10卷 3621-3628页

作者： Yue Qi chun-ting he Juntao Lin Shuping Lin Jin Liu Jinghong Huang Wei Xue Guicheng Yu Hsiu-Yi Chao Yexiang Tong Zhengping Qiao MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China

Nanoscale metal-organic frameworks （NMOFs） have attracted increased attention in recent years for miniaturized and/or biological ***,the synthesis of ultrasmall NMOFs with good stability is a great *** this study,sub-5-nm nano-HKUST-1 was prepared for the first time via a mild metalorganic gel route without surfactants or capping *** the gelation process via anion-ligand self-assembly is the key to the formation of *** Tyndall effect,zeta potential,and liquid adsorption indicated strong stability of the obtained nano-HKUST-1,even in *** experiments were performed using different dyes （crystal violet and methylene blue） to demonstrate the size-dependent adsorption thermodynamics and kinetics of this famous *** results of this study provide new insights regarding the synthesis of NMOFs and their efficient applications.

关键词： metal-orgamc gel metal-organic frameworks nanoparticles,liquid adsorption

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A Crystalline Supramolecular Rotor Functioned by Dual Ultrasmall Polar Rotators

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Chinese Journal of Chemistry 2022年第16期40卷 1917-1923页

作者： Wang Li De-Xuan Liu Wei-Yu Hu Qing-Yan Liu Zi-Yi Du chun-ting he Wei-Xiong Zhang Xiao-Ming Chen College of Chemistry and Chemical Engineering MOE Key Laboratory of Fluorine and Silicon for Energy Materials and ChemistryJiangxi Normal UniversityNanchangJiangxi330022 China School of Chemistry MOE Key Laboratory of Bioinorganic and Synthetic ChemistrySun Yat-Sen UniversityGuangzhouGuangdong510275 China

As an extended model of conventional molecular rotors,a conceived construction of novel crystalline molecular rotor that simultaneously contains two discrete polar rotators is presented *** supramolecular self-assembly of 18-crown-6 host and two rotator-containing ion-pair guests affords a three-in-one cocrystal,(2-NH_(3)-iBuOH)(18-crown-6)[ZnBr_(3)(H_(2)O)],in which the hydroxyl group and aqua ligand both function as ultrasmall polar *** the basis of the variable-temperature single-crystal X-ray diffraction,variable-temperature/frequency dielectric response,density functional theory calculations,and molecular dynamics simulations,it is found that such dual polar rotators experience a gradually enhanced rotation with increasing temperature,and more importantly,could be controlled by a reversible polar-to-polar structural phase transition,i.e.,from a“single-(polar rotator)”state at low-temperature phase to a“mixed-dual-(polar rotator)”state in the vicinity of transition,and to an unusual“synchronized-dual-(polar rotator)”state at high-temperature phase.

关键词： Molecular rotor Host-guest system Dielectric relaxation Molecular dynamics Phase transition

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A gating ultramicroporous metal-organic framework showing high adsorption selectivity,capacity and rate for xylene separation

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Science China Chemistry 2022年第8期65卷 1552-1558页

作者： Zi-Ming Ye Xue-Feng Zhang De-Xuan Liu Yan-Tong Xu Chao Wang Kai Zheng Dong-Dong Zhou chun-ting he Jie-Peng Zhang Key Laboratory of Bioinorganic and Synthetic Chemistry(Ministry of Education) School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis Jiangxi Normal UniversityNanchang 330022China 3.Guangdong Provincial Key Laboratory of New and Renewable Energy Research and DevelopmentGuangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China

Adsorptive separation of p-xylene(pX)from xylene isomers is a key process in chemical industry,but known adsorbents cannot simultaneously achieve high adsorption selectivity,capacity,and ***,we demonstrate gating ultramicropore as a solution for this *** modification of the synthetic condition gives rise to isomeric metal-organic frameworksα-[Zn(pba)](MAF-88,H2pba=4-(1H-pyrazol-4-yl)benzoic acid)andβ-[Zn(pba)](MAF-89)possessing similar pillared-column structures,porosities,and high pX capacities of 2.0 mmol g^(−1),but very different framework/pore topologies,pore sizes,and pX *** binary and ternary mixtures of liquid xylene isomers,MAF-88 with narrow one-dimensional(1D)channels shows pX selectivity of 11 and 1.6,while MAF-89 with 3D-connected quasi-discrete pores shows pX selectivity up to 221 and 46,***,differential scanning calorimetry,and time-dependent separation experiments reveal that the kinetic effects of the gating pores play more important roles than the thermodynamic effects,which is further confirmed by single-crystal X-ray diffraction and computational simulations.

关键词： metal-organic frameworks gating xylene adsorption separation

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Disclosing the active integration structure and robustness of a pseudo-tri-component electrocatalyst toward alkaline hydrogen evolution

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Journal of Energy Chemistry 2022年第9期31卷 210-216,I0007页

作者： Hong-Hong Zou Wan-Qing Li Cong-Hu Song Li-Ming Cao Xue-Feng Zhang Xuan-Yi Zhu Zi-Yi Du Jia Zhang Sheng-Liang Zhong chun-ting he Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education and College of Life ScienceJiangxi Normal UniversityNanchang 330022JiangxiChina Research Center for Ultrafine Powder Materials College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022JiangxiChina

Designing multicomponent integration catalysts(MICs)has been a promising strategy for improving electrocatalytic hydrogen evolution reaction(heR)due to the highly active interfaces as well as electronic ***,many fundamental questions such as their actual active species and the influence on long-term stability remain to be ***,we present the structural evolution from a pseudotri-component electrocatalyst of nitrogen-doped carbon supported nickel/vanadium nitride/vanadium oxide(Ni-VN-V_(2)O_(3)/NC)nanorods to the heterostructural nickel/vanadium nitride(Ni-VN/NC)nanosheets during chemical or electrochemical *** self-reconstructed Ni-VN/NC exhibits a robust stability under alkaline conditions,while maintaining initial efficient heR activity with a low overpotential of 76 mV at the current density of 10 mA cm^(-2).Theoretical calculations and quasi-in-situ spectroscopic technology unveil the redistribution of electrons on the synergistic active interface,which synchronously optimizes the affinities for hydrogen,hydroxide,and water molecules,thereby remarkably accelerating the heR kinetics by reducing the barrier of Volmer step.

关键词： Hydrogen evolution reaction Multicomponent integration catalysts Structural transformation Electrocatalysis Density functional theory

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