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Manipulating the Morphology and Electronic State of a Two-Dimensional Coordination Polymer as a Hydrogen Evolution Cocatalyst Enhances Photocatalytic Overall Water Splitting
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-01-09 , DOI: 10.1021/acscatal.3c04389 Jingyan Guan 1 , Kazuma Koizumi 2 , Naoya Fukui 3 , Hajime Suzuki 1 , Kantaro Murayama 1 , Ryojun Toyoda 2 , Hiroaki Maeda 3 , Kazuhide Kamiya 4, 5 , Keitaro Ohashi 4 , Shinya Takaishi 2 , Osamu Tomita 1 , Akinori Saeki 5, 6 , Hiroshi Nishihara 3 , Hiroshi Kageyama 1 , Ryu Abe 1 , Ryota Sakamoto 2, 7
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-01-09 , DOI: 10.1021/acscatal.3c04389 Jingyan Guan 1 , Kazuma Koizumi 2 , Naoya Fukui 3 , Hajime Suzuki 1 , Kantaro Murayama 1 , Ryojun Toyoda 2 , Hiroaki Maeda 3 , Kazuhide Kamiya 4, 5 , Keitaro Ohashi 4 , Shinya Takaishi 2 , Osamu Tomita 1 , Akinori Saeki 5, 6 , Hiroshi Nishihara 3 , Hiroshi Kageyama 1 , Ryu Abe 1 , Ryota Sakamoto 2, 7
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To achieve efficacious photocatalytic overall water splitting, surface modification of photocatalysts with proficient cocatalysts for hydrogen evolution reaction (HER) is imperative. NiBHT, a conductive two-dimensional coordination polymer (2D CP), or a 2D metal–organic framework (2D MOF), endowed with remarkable chemical stability and HER selectivity, emerged as a promising candidate for an HER cocatalyst. However, the bulky morphology of NiBHT hampered its performance. Here, we demonstrate a strategy to miniaturize NiBHT by incorporating the benzene-1,2-dithiol (BDT) ligand, yielding NiBHT nanoparticles (NiBHT-NP). Beyond morphology, empirical evidence unveiled alterations in the electronic state and catalytic activity of NiBHT-NP, and the ramifications of BDT modulation on intrinsic characteristics are elucidated through density functional theory (DFT) calculations. As a model system, CoOx/SrTiO3:Al photocatalyst with NiBHT-NP modification exhibited an apparent quantum efficiency (AQE) of 10.3% at 365 nm for overall water splitting. This pioneering work showcases that a modulator ligand may manipulate the morphology, electronic state, and catalytic behavior of 2D CPs, holding prodigious potential for developing more effective CP-based HER cocatalysts.
中文翻译：
操纵二维配位聚合物的形态和电子态作为析氢助催化剂增强光催化整体水分解
为了实现有效的光催化整体水分解，必须使用高效的析氢反应（HER）助催化剂对光催化剂进行表面改性。NiBHT 是一种导电二维配位聚合物 (2D CP) 或二维金属有机骨架 (2D MOF)，具有显着的化学稳定性和 HER 选择性，成为 HER 助催化剂的有前途的候选者。然而，NiBHT 的庞大形貌阻碍了其性能。在这里，我们展示了一种通过掺入苯-1,2-二硫醇（BDT）配体来小型化 NiBHT 的策略，产生 NiBHT 纳米颗粒（NiBHT-NP）。除了形态之外，经验证据还揭示了 NiBHT-NP 电子态和催化活性的变化，并且通过密度泛函理论 (DFT) 计算阐明了 BDT 调制对内在特征的影响。作为模型系统，NiBHT-NP 改性的 CoO x /SrTiO 3 :Al 光催化剂在 365 nm 处表现出 10.3% 的总水分解表观量子效率 (AQE)。这项开创性的工作表明，调节剂配体可以操纵 2D CP 的形态、电子态和催化行为，为开发更有效的基于 CP 的 HER 助催化剂拥有巨大的潜力。
更新日期：2024-01-09
中文翻译：
操纵二维配位聚合物的形态和电子态作为析氢助催化剂增强光催化整体水分解
为了实现有效的光催化整体水分解，必须使用高效的析氢反应（HER）助催化剂对光催化剂进行表面改性。NiBHT 是一种导电二维配位聚合物 (2D CP) 或二维金属有机骨架 (2D MOF)，具有显着的化学稳定性和 HER 选择性，成为 HER 助催化剂的有前途的候选者。然而，NiBHT 的庞大形貌阻碍了其性能。在这里，我们展示了一种通过掺入苯-1,2-二硫醇（BDT）配体来小型化 NiBHT 的策略，产生 NiBHT 纳米颗粒（NiBHT-NP）。除了形态之外，经验证据还揭示了 NiBHT-NP 电子态和催化活性的变化，并且通过密度泛函理论 (DFT) 计算阐明了 BDT 调制对内在特征的影响。作为模型系统，NiBHT-NP 改性的 CoO x /SrTiO 3 :Al 光催化剂在 365 nm 处表现出 10.3% 的总水分解表观量子效率 (AQE)。这项开创性的工作表明，调节剂配体可以操纵 2D CP 的形态、电子态和催化行为，为开发更有效的基于 CP 的 HER 助催化剂拥有巨大的潜力。
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