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Electronic Regulation of Pt Single-Atom Catalysts via Local Coordination State Adjustment for Enhanced Photocatalytic Performance
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-06-01 , DOI: 10.1021/acscatal.3c01141 Huanhuan Zhai 1 , Pengfei Tan 1 , Min Jiang 1 , Mingyuan Zhang 1 , Ruifeng Ren 1 , Rongjian Sa 2 , Jun Pan 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-06-01 , DOI: 10.1021/acscatal.3c01141 Huanhuan Zhai 1 , Pengfei Tan 1 , Min Jiang 1 , Mingyuan Zhang 1 , Ruifeng Ren 1 , Rongjian Sa 2 , Jun Pan 1
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Single-atom catalysts (SACs) are deemed as the ultimate ceiling route to release the full potential of metal utilization efficiency, while the tougher challenge is to optimize the microstructure for motivating the photocatalytic activity to move forward. Here, Pt SACs with Pt–C2N and Pt–N2 configurations are synthesized by regulating the N vacancy level of ultrathin g-C3N4 (UCN). The distinctive configuration of Pt–C2N and Pt–N2 has been confirmed by X-ray absorption fine spectroscopy. Surprisingly, Pt–C2N displays a satisfactory H2 evolution performance of 112.5 μmol h–1, which is higher than that of Pt–N2 (78.6 μmol h–1). The underlying origins of the discrepancy are investigated by density functional theory (DFT) calculations, which detect that Pt atoms are apt to absorb on C2C to construct strong metal–support interactions. Particularly, owing to the reduced H* desorption energy and a short carrier delivery channel for Pt–C2N, H+ could readily couple with abundant electrons during the hydrogen evolution reaction (HER). Our work points out the future directions for the enhancement of photocatalytic performance by regulating the geometric and electronic structures.
中文翻译：
通过局部配位态调整对 Pt 单原子催化剂进行电子调控以提高光催化性能
单原子催化剂 (SAC) 被认为是释放金属利用效率全部潜力的终极途径，而更严峻的挑战是优化微观结构以激发光催化活性向前发展。在这里，通过调节超薄 gC 3 N 4 (UCN)的 N 空位水平合成具有Pt–C 2 N 和 Pt–N 2构型的 Pt SAC 。Pt-C 2 N 和 Pt-N 2的独特构型已通过 X 射线吸收精细光谱得到证实。令人惊讶的是， Pt –C 2 N 表现出令人满意的112.5 μmol h –1 析氢性能，高于 Pt–N2 (78.6 μmol·h –1 )。通过密度泛函理论 (DFT) 计算研究了差异的根本原因，该计算检测到 Pt 原子易于吸收在 C 2C上以构建强金属-载体相互作用。特别是，由于 Pt-C 2 N 的 H* 解吸能降低和载流子输送通道较短，H +在析氢反应 (HER) 过程中很容易与丰富的电子耦合。我们的工作指出了通过调节几何和电子结构来提高光催化性能的未来方向。
更新日期：2023-06-01
中文翻译：
通过局部配位态调整对 Pt 单原子催化剂进行电子调控以提高光催化性能
单原子催化剂 (SAC) 被认为是释放金属利用效率全部潜力的终极途径，而更严峻的挑战是优化微观结构以激发光催化活性向前发展。在这里，通过调节超薄 gC 3 N 4 (UCN)的 N 空位水平合成具有Pt–C 2 N 和 Pt–N 2构型的 Pt SAC 。Pt-C 2 N 和 Pt-N 2的独特构型已通过 X 射线吸收精细光谱得到证实。令人惊讶的是， Pt –C 2 N 表现出令人满意的112.5 μmol h –1 析氢性能，高于 Pt–N2 (78.6 μmol·h –1 )。通过密度泛函理论 (DFT) 计算研究了差异的根本原因，该计算检测到 Pt 原子易于吸收在 C 2C上以构建强金属-载体相互作用。特别是，由于 Pt-C 2 N 的 H* 解吸能降低和载流子输送通道较短，H +在析氢反应 (HER) 过程中很容易与丰富的电子耦合。我们的工作指出了通过调节几何和电子结构来提高光催化性能的未来方向。
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