Manipulating the Morphology and Electronic State of a Two-Dimensional Coordination Polymer as a Hydrogen Evolution Cocatalyst Enhances Photocatalytic Overall Water Splitting

Jingyan Guan, Kazuma Koizumi, Naoya Fukui, Hajime Suzuki, Kantaro Murayama, Ryojun Toyoda, Hiroaki Maeda, Kazuhide Kamiya, Keitaro Ohashi, Shinya Takaishi, Osamu Tomita, Akinori Saeki, Hiroshi Nishihara, Hiroshi Kageyama, Ryu Abe, Ryota Sakamoto

研究成果: ジャーナルへの寄稿学術論文査読

14 被引用数 (Scopus)

抄録

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.

本文言語英語
ページ(範囲)1146-1156
ページ数11
ジャーナルACS Catalysis
14
2
DOI
出版ステータス出版済み - 2024 1月 19

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