CeO_(2)-Cu_(2)O_(2)D/3D S型异质结界面促进有序电荷转移以实现高效光催化析氢  

2D/3D S-Scheme Heterojunction Interface of CeO_(2)-Cu_(2)O Promotes Ordered Charge Transfer for Efficient Photocatalytic Hydrogen Evolution

作　　者：张利君 吴有林 Noritatsu Tsubaki 靳治良[1] Lijun Zhang;Youlin Wu;Noritatsu Tsubaki;Zhiliang Jin(School of Chemistry and Chemical Engineering,North Minzu University,Yinchuan 750021,China;Department of Applied Chemistry,Graduate School of Engineering,University of Toyama,Gofuku 3190,Toyama 930-8555,Japan.)

机构地区：[1]北方民族大学化学与化学工程学院,银川750021 [2]富山大学工学部,应用化学系,五福3190,富山930-8555,日本

出　　处：《物理化学学报》2023年第12期145-154,共10页Acta Physico-Chimica Sinica

基　　金：国家自然科学基金(22062001);宁夏废弃食用油转化为清洁能源高附加值化学品创新团队和低品位资源高值化利用及环境化工一体化技术创新团队资助项目。

摘　　要：快速的本征载流子复合严重限制了CeO_(2)基催化材料的光催化活性。在这里,提出了一种异质结界面工程策略,合理地进行界面调节。构建了具有强电子相互作用的2D/3D S型异质结。合成了一种用于固定在2D CeO_(2)边缘的3D Cu_(2)O颗粒的复合光催化剂。密度泛函理论(DFT)第一性原理计算和实验结果表明,CeO_(2)和Cu_(2)O之间形成强耦合的S型异质结电子传输界面,实现了高效的载流子分离和传输。复合催化剂的光催化析氢活性在以三乙醇胺为牺牲剂的体系中得到大幅提高,是CeO_(2)的48倍。此外,CeO_(2)-Cu_(2)O光催化剂还具有高度稳定的光催化氢活性。这为在新型纳米复合结构中构建独特界面提供了一种通用策略。Rapid intrinsic carrier recombination severely restricts the photocatalytic activity of CeO_(2)-based catalytic materials.In this study,a heterogeneous interfacial engineering strategy is proposed to rationally perform interface modulation.A 2D/3D Sscheme heterojunction with strong electronic interactions was constructed.A composite photocatalyst was synthesized for the 3D Cu_(2)O particles anchored at the edge of 2D CeO_(2).Firstprinciples calculations(based on density functional theory)and the experimental results show that a strongly coupled S-scheme heterojunction electron transport interface is formed between CeO_(2) and Cu_(2)O,resulting in efficient carrier separation and transfer.The photocatalytic hydrogen evolution activity of the composite catalyst is significantly improved in the system with triethanolamine as the sacrificial agent and is 48 times as that of CeO_(2).In addition,the resulting CeO_(2)-Cu_(2)O photocatalyst affords highly stable photocatalytic hydrogen activity.This provides a general technique for constructing unique interfaces in novel nanocomposite structures.

关 键 词：CeO_(2) Cu_(2)O DFT S型异质结 光催化析氢 

分 类 号：O643[理学—物理化学]