Functionalization has emerged as a pivotal endeavor to tailor the surface properties of photocatalysts. We propose a facile amine functionalization strategy to establish a Cu−In−Zn−S (CIZS)/NiS x hybrid with covalent bonds using individual ethylenediamine (EDA) molecules. Our approach witnesses a remarkable photocatalytic hydrogen evolution (PHE) competence of 65.93 mmol g −1 h −1 driven by visible light, the highest value yielded by CIZS to date. X-ray absorption spectra of CIZS and density functional theory (DFT) calculations confirm the crucial amine N→Cu coordination after amine functionalization. The new emerging coordination via lone-pair electron donation profitably accesses the regulation of the coordination environment, electronic structures, and carrier behavior. Moreover, individual EDA molecule with two-terminal −NH 2 group serves as a molecular bridge to hybrid CIZS and NiS x cocatalyst via N→Cu and N→Ni coordination, favorably promoting efficient charge transport. This study provides advances in practical functionalizing photocatalysts.
Jinghui Wang,Renliang Huang,Wei Qi,Rongxin Su,Zhimin He
In spite of the rapid development of nanozyme, it is still challenging to develop multifunctional nanozyme with high oxidase-like activity. In this work, a novel type of amorphous MOF based nanozyme (CA-Cu) with both laccase- and catecholase-like activity was prepared by the facile solvothermal reaction of cyanuric acid and Cu 2+ to mimick the N-Cu coordinated environment between the imidazole and Cu 2+ in their active site. Due to the excellent activity, substrate universality, recyclability and stability of CA-Cu nanozyme, it shows broad application prospects in degradation and detection of phenolic compounds. Besides, the structure–activity relationship between N-Cu coordinated environment and laccase/catecholase-like activity has been further proved.
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