Rational Design of Three Dimensional Hollow Heterojunctions for Efficient Photocatalytic Hydrogen Evolution Applications

Author:

Pan Jingwen1,Wang Dongbo1ORCID,Wu Donghai2,Cao Jiamu3,Fang Xuan4,Zhao Chenchen1,Zeng Zhi1,Zhang Bingke1,Liu Donghao1,Liu Sihang1,Liu Gang5,Jiao Shujie1,Xu Zhikun6,Zhao Liancheng1,Wang Jinzhong1

Affiliation:

1. School of Materials Science and Engineering Harbin Institute of Technology Harbin 150001 China

2. Henan Key Laboratory of Nanocomposites and Applications Huanghe Science and Technology College Institute of Nanostructured Functional Materials Zhengzhou 450006 China

3. School of Astronautics Harbin Institute of Technology Harbin 150001 China

4. State Key Lab High Power Semicond Lasers Changchun University Science and Technology, Sch Sci Changchun 130022 China

5. Center for High Pressure Science and Technology Advanced Research Shanghai 201203 China

6. Guangdong University of Petrochemical Technology Maoming 525000 China

Abstract

AbstractThe efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Publisher

Wiley

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