Heterobimetallic[NiCo]integration in a hydrogenase mimic for boosting light-driven hydrogen evolution in CaTiO_(3)  

作　　者：Kang Li Juanji Hong Ningning Song Zhanjun Guo Minmin Liang 

机构地区：[1]Experimental Center of Advanced Materials,School of Materials Science&Engineering,Beijing Institute of Technology,Beijing 10081,China

出　　处：《Nano Research》2024年第8期6888-6894,共7页纳米研究（英文版）

基　　金：supported by the National Key R&D Program of China(No.2022YFA1205801);the National Natural Science Foundation of China(Nos.T2225026,82172087,82071308,and 52202344);Beijing Institute of Technology Research Fund Program for Young Scholars.

摘　　要：Light-drive hydrogen production using titanium-based perovskite is one sustainable way to reduce current reliance on fossil fuels,but its wide applications are still limited by high electron−hole recombination and sluggish surface reaction.Thus,the developments for low-cost and highly efficient co-catalysts remain urgent.Inspired by natural[NiFe]-hydrogenase active center structure,a hydrogenase-mimic,NiCo_(2)S_(4) nanozyme was synthesized,and subsequently decorated onto the CaTiO_(3) to catalyze the hydrogen evolution reaction(HER).Among the following test,CaTiO_(3)with a 15%loading of NiCo_(2)S_(4) nanozyme exhibited the highest HER rate of 307.76μmol·g^(–1)·h^(–1),which is 60 times higher than that of the CaTiO_(3) alone.The results reveal that NiCo_(2)S_(4) not only significantly increased the charge separation efficiency of the photogenerated carriers,but also substantively lowered the HER activation energy.Mechanism studies show that NiCo_(2)S_(4) readily splits H_(2)O by forming the Ni(OH)-Co intermediate and only Ni in the bimetallic center alters the oxidation state during the HER process in a manner analogous to the[NiFe]-hydrogenase.In contrast to the often-expensive synthetic catalysts that rely on rare elements such as ruthenium and platinum,this study shows a promising way to develop the nature-inspired cocatalysts to enhance the photocatalysts’HER performance.

关 键 词：hydrogen evolution reaction hydrogenase-mimic nanozyme PHOTOCATALYST WATER-SPLITTING 

分 类 号：O64[理学—物理化学]