Design and fabrication of a novel 2D/3D ZnIn2S4@Ni1/UiO-66-NH2 heterojunction for highly efficient visible-light photocatalytic H2 evolution coupled with benzyl alcohol valorization

• Published in: Applied catalysis. B, Environmental Vol. 357; p. 124279
• Main Authors: Jia, Zhiwen, Li, Rong, Ji, Peizhu, Xu, Zining, Homewood, Kevin Peter, Xia, Xiaohong, Gao, Yun, Zou, Jian-Ping, Chen, Xuxing
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 15.11.2024
• Subjects: Photocatalytic H2 production; Selective alcohol oxidation; Single-atom catalyst; UiO-66-NH2; ZnIn2S4; UiO-66-NH2; Photocatalytic H2 production; Single-atom catalyst; ZnIn2S4; Selective alcohol oxidation
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2024.124279

Making full use of photogenerated charge carriers by careful design multifunctional photocatalysts to achieving bi-value-added production with high-efficiency is highly desirable and extremely challenge. Herein, a novel 2D/3D ZnIn2S4@Ni1/UiO-66-NH2 (ZIS@Ni1/UN) heterojunction with spatially separated and precise redox sites was designed and fabricated for both photocatalytic H2 production and benzyl alcohol (BA) valorization. By precise structural regulation and modification of UiO-66 integrated with -NH2, ZnIn2S4 (ZIS) and Ni single-atom, the spatial separation of redox sites and directional electron transfer has been achieved. This realizes collaborative and efficient solar energy to chemical energy conversion. The optimal sample 5ZIS@Ni1/UN-6 shows high photocatalytic H2 and benzaldehyde (BAD) production rates of 11.44 mmol∙g−1∙h−1 and 10.02 mmol∙g−1∙h−1 under visible light. This work highlights the importance of rational construction for the engineering of charge behavior in heterogeneous photocatalysts with spatial separation and identifies their crucial role in promoting the photocatalytic redox coupling reactions. [Display omitted] •A novel 2D/3D ZnIn2S4@Ni1/UiO-66-NH2 heterojunction is successfully design and fabricated.•High production rates of benzaldehyde and H2 simultaneous is achieved under visible-light.•Precise construction of spatially separated redox-sites and directional electron transfer synergistically boost photocatalytic performance.•The carbon-centered free radical process of selective oxidation of benzylalcohol is confirmed by in-situ EPR.