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CoFe MOF衍生的双金属氢氧化物助催化剂促进稳定的太阳能水分解OA北大核心CSTPCD

Bimetallic Oxyhydroxide Cocatalyst Derived from CoFe MOF for Stable Solar Water Splitting

中文摘要英文摘要

金属有机骨架(MOFs)作为一种高效的电催化剂,在光电化学中具有广阔的应用前景.在此,我们开发了一种将金属有机框架作为析氧助催化剂(OEC)与半导体相结合的策略,以改善电荷传输并减少体/表面载流子复合.制备的CoFe MOF/BiVO4光阳极在AM 1.5G照明下,1.23 V(vs.RHE)下表现出4.5 mA·cm-2的光电流密度,实现了卓越的长期光稳定性.值得注意的是,随着MOF在长期水氧化反应中的重建,BiVO4表面形成了更稳定的金属氢氧化物,光电极的光电流密度进一步提高到5 mA·cm-2.根据密度泛函理论计算,光电化学(PEC)性能的提高可归因于Co和Fe之间的耦合效应,降低了自由能垒并加速了反应动力学.本工作的重点是在长期水氧化过程中,将CoFe MOF催化剂重新构建为双金属氢氧化物.本文通过设计MOFs催化剂和构筑高效稳定的光阳极,开发了一种有效且可行的PEC水分解的途径.

Metal-organic frameworks(MOFs)as efficient electrocatalysts can be employed as the promising cocatalysts in photoelectrochemistry.Herein,a strategy is developed to metal-organic frameworks as oxygen evolution cocatalyst(OEC)combined with semiconductor for improving the charge transport and reducing the bulk/surface carrier recombination.This advanced CoFe MOF/BiVO4 photoanode exhibits a photocurrent density of 4.5 mA∙cm-2 at 1.23 V(vs.RHE)under AM 1.5G illumination,achieving outstanding long-term photostability.Remarkably,with the reconstruction of MOF in the long-term water oxidation reaction,more stable metal oxyhydroxides are formed on the surface of BiVO4 and the photocurrent density of the photoelectrode is further enhanced to 5 mA∙cm-2.From density functional theory calculations,the enhanced photoelectrochemical(PEC)performance can be attributed to the coupling effect between Co and Fe decreasing the free energy barriers and accelerating the reaction kinetics.This work focuses on the reconfiguration of CoFe MOF catalyst to bimetallic hydroxide during long-term water oxidation.This work enables us to develop an effective pathway to design and fabricate efficient and stable photoanodes through MOFs catalysts for feasible PEC water splitting.

任世杰;高明泽;高瑞廷;王蕾

内蒙古大学化学化工学院,能源材料化学研究院,呼和浩特 010021

化学

CoFe MOF太阳能水分解表面改性表面重建BiVO4

CoFe MOFSolar water splittingSurface modificationSurface reconstructionBiVO4

《物理化学学报》 2024 (007)

47-49 / 3

The work was supported by the National Key Research and Development Program of China(2022YFA1205200)and the National Natural Science Foundation of China(21965024,22269016).中国国家重点研究发展计划(2022YFA1205200)和国家自然科学基金(21965024,22269016)资助项目

10.3866/PKU.WHXB202307040

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