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用于促进光催化析氢的石墨相氮化碳纳米片上的原子精确Ni(SCHPh)纳米团簇

Atomically precise Ni(SCHPh) nanoclusters on graphitic carbon nitride nanosheets for boosting photocatalytic hydrogen evolution.

作者信息

Wei Jieding, Zhao Renqiang, Luo Dian, Lu Xiangyu, Dong Wenxiu, Huang Yucheng, Cheng Xiaomei, Ni Yonghong

机构信息

College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, PR China.

College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, PR China.

出版信息

J Colloid Interface Sci. 2023 Feb;631(Pt A):212-221. doi: 10.1016/j.jcis.2022.11.010. Epub 2022 Nov 9.

DOI:10.1016/j.jcis.2022.11.010
PMID:36375301
Abstract

Much effort has been devoted to improving the photocatalytic capacity of graphitic carbon nitride (g-CN). In this paper, we reported the successful synthesis of a hybrid photocatalyst with superb photocatalytic hydrogen production activity through decorating atomically precise Ni(SCHPh) nanoclusters on g-CN nanosheets (labeled as Ni/g-CN) at room temperature. Zeta potential experiments demonstrated that the electrostatic interaction between Ni and g-CN led to the formation of Ni/g-CN. The photocatalytic measurements revealed that the 5 %-Ni/g-CN prepared with the original mass ratio of m(Ni)/m(g-CN) = 1/20 exhibited the strongest hydrogen production activity. In the system with triethanolamine (TEOA) as the sacrifice agent, the visible-light hydrogen production rate reached up to 5.87 mmol h g, approximately 290 times higher than that of pure g-CN (0.02 mmol h g). Density functional theory (DFT) calculations testified that the above significant enhancement of photocatalytic hydrogen evolution of the hybrid photocatalyst arose from the photogenerated electrons transfer from Ni to g-CN.

摘要

人们已付出诸多努力来提高石墨相氮化碳(g-CN)的光催化能力。在本文中,我们报道了通过在室温下将原子精确的Ni(SCHPh)纳米团簇修饰在g-CN纳米片上(标记为Ni/g-CN),成功合成了一种具有卓越光催化产氢活性的复合光催化剂。zeta电位实验表明,Ni与g-CN之间的静电相互作用导致了Ni/g-CN的形成。光催化测量结果显示,以m(Ni)/m(g-CN)=1/20的原始质量比制备的5%-Ni/g-CN表现出最强的产氢活性。在以三乙醇胺(TEOA)作为牺牲剂的体系中,可见光产氢速率高达5.87 mmol h g,约为纯g-CN(0.02 mmol h g)的290倍。密度泛函理论(DFT)计算证明,上述复合光催化剂光催化析氢的显著增强源于光生电子从Ni向g-CN的转移。

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