State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
Department of Physics and CSRRI, Illinois Institute of Technology, Chicago, IL, 60616, USA.
Angew Chem Int Ed Engl. 2023 Jun 19;62(25):e202217439. doi: 10.1002/anie.202217439. Epub 2023 Apr 3.
A photocatalyst TiO /Ti-BPDC-Pt is developed with a self-grown TiO /Ti-metal-organic framework (MOF) heterojunction, i.e., TiO /Ti-BPDC, and selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC for photocatalytic hydrogen evolution. This intimate heterojunction, growing from the surface pyrolytic reconstruction of Ti-BPDC, works in a direct Z-scheme, efficiently separating electrons and holes. Pt is selectively anchored on Ti-BPDC by ligands and is found in the form of single atoms with loading up to 1.8 wt %. The selective location of Pt is the electron-enriched domain of the heterojunction, which further enhances the utilization of the separated electrons. This tailored TiO /Ti-BPDC-Pt shows a significantly enhanced activity of 12.4 mmol g h compared to other TiO - or MOF-based catalysts. The structure-activity relationship further proves the balance of two simultaneously exposed domains of heterojunctions is critical to fulfilling this kind of catalyst.
开发了一种光催化剂 TiO /Ti-BPDC-Pt，它具有自生长的 TiO /Ti-金属-有机骨架（MOF）异质结，即 TiO /Ti-BPDC，并选择性地在 Ti-BPDC 上锚定高密度 Pt 单原子助催化剂用于光催化析氢。这种从 Ti-BPDC 的表面热解重构中生长出来的紧密异质结以直接 Z 方案工作，有效地分离电子和空穴。Pt 通过配体选择性地锚定在 Ti-BPDC 上，以负载量高达 1.8wt%的形式存在于单原子形式中。Pt 的选择性位置是异质结的电子富域，进一步增强了分离电子的利用。这种定制的 TiO /Ti-BPDC-Pt 的活性明显提高，达到 12.4mmol g -1 h -1，优于其他 TiO 或 MOF 基催化剂。结构-活性关系进一步证明，异质结的两个同时暴露的域之间的平衡对于实现这种催化剂至关重要。
