Construction of Six‐Oxygen‐Coordinated Single Ni Sites on g‐C3N4 with Boron‐Oxo Species for Photocatalytic Water‐Activation‐Induced CO2 Reduction

材料科学 催化作用 光催化 吸附 Atom(片上系统) 光化学 氧气 X射线光电子能谱 水溶液 化学工程 物理化学 化学 有机化学 嵌入式系统 工程类 计算机科学
作者
Yuying Wang,Yang Qu,Binhong Qu,Linlu Bai,Yang Liu,Zhao‐Di Yang,Wei Zhang,Liqiang Jing,Honggang Fu
出处
期刊:Advanced Materials [Wiley]
卷期号:33 (48) 被引量:192
标识
DOI:10.1002/adma.202105482
摘要

Abstract The configuration regulation of single‐atom photocatalysts (SAPCs) can significantly influence the interfacial charge transfer and subsequent catalytic process. The construction of conventional SAPCs for aqueous CO 2 reduction is mainly devoted toward favorable activation and photoreduction of CO 2 , however, the role of water is frequently neglected. In this work, single Ni atoms are successfully anchored by boron‐oxo species on g‐C 3 N 4 nanosheets through a facile ion‐exchange method. The dative interaction between the B atom and the sp 2 N atom of g‐C 3 N 4 guarantees the high dispersion of boron‐oxo species, where O atoms coordinate with single Ni (II) sites to obtain a unique six‐oxygen‐coordinated configuration. The optimized single‐atom Ni photocatalyst, rivaling Pt‐modified g‐C 3 N 4 nanosheets, provides excellent CO 2 reduction rate with CO and CH 4 as products. Quasi‐in‐situ X‐ray photoelectron spectra, transient absorption spectra, isotopic labeling, and in situ Fourier transform infrared spectra reveal that as‐fabricated six‐oxygen‐coordinated single Ni (II) sites can effectively capture the photoelectrons of CN along the BO bridges and preferentially activate adsorbed water to produce H atoms to eventually induce a hydrogen‐assisted CO 2 reduction. This work diversifies the synthetic strategies for single‐atom catalysts and provides insight on correlation between the single‐atom configuration and reaction pathway.
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