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

IF 13.5 2区化学 Q1 CHEMISTRY, PHYSICAL 物理化学学报 Pub Date : 2024-07-01 Epub Date: 2023-08-31 DOI:10.3866/PKU.WHXB202307040

Shijie Ren , Mingze Gao , Rui-Ting Gao, Lei Wang

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Abstract

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.

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由CoFe MOF衍生的双金属氢氧化物助催化剂用于稳定的太阳能水分解

金属有机骨架作为高效的电催化剂，在光电化学领域具有广阔的应用前景。本文提出了一种将金属-有机骨架作为析氧助催化剂（OEC）与半导体相结合的策略，以改善电荷输运并减少体/表面载流子的复合。这种先进的CoFe MOF/BiVO4光阳极在AM 1.5G照明下，在1.23 V （vs. RHE）下的光电流密度为4.5 mA·cm−2，具有出色的长期光稳定性。值得注意的是，在长期的水氧化反应中，随着MOF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。密度泛函理论计算表明，Co和Fe之间的耦合作用降低了自由能垒，加速了反应动力学，从而增强了电化学性能。研究了长期水氧化过程中CoFe - MOF催化剂向双金属氢氧化物的重构。这项工作使我们能够开发出一种有效的途径，通过mof催化剂设计和制造高效稳定的光阳极，用于可行的PEC水分解。下载：下载高分辨率图片（62KB）下载：下载全尺寸图片

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