钌单原子修饰在联苯上增强析氢反应的DFT研究

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2025-09-26 DOI:10.1039/d5cp02045j

Sun Shikai, Manman Liu, David J. Singh, Wei Tao Zheng, Xiaofeng Fan

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引用次数: 0

摘要

开发高效、经济、耐用的析氢反应电催化剂是实现可持续氢能的基石。然而，高效、低成本的HER催化剂仍然非常有限。在这项研究中，我们采用自旋极化密度泛函理论计算来研究钌（Ru）单原子催化剂（SACs）锚定在联苯（BPN）底物上的催化性能。发现BPN独特的二维结构和电子特性为隔离金属原子提供了一个有前途的平台。发现Ru原子优先锚定在C₄中空位点，产生-0.093 eV的ΔGH*，与Pt上的H（111）相当。此外，双Ru修饰BPN （2Ru-BPN）能量稳定，可作为双原子催化剂（dac）。2Ru-BPN中的活性基团可导致多氢吸附，吉布斯自由能变化约为-0.12 eV，从而促进H在热中性条件下沿Tafel途径演化。因此，这项工作为设计高性能ru基sac提供了理论蓝图，并增强了BPN作为下一代制氢催化剂载体的潜力。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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Enhanced Hydrogen Evolution Reaction Catalysis via Ruthenium Single-Atom Decoration on Biphenylene: A DFT Study

The development of efficient, cost-effective, and durable electro-catalysts for the hydrogen evolution reaction (HER) remains a cornerstone for realizing sustainable hydrogen energy. However, the highly efficient catalysts with low cost for HER are still very limited. In this study, we employ spin-polarized density functional theory calculations to investigate the catalytic performance of ruthenium (Ru) single-atom catalysts (SACs) anchored on a biphenylene (BPN) substrate. It is found that the unique two-dimensional architecture and electronic characteristics of BPN offer a promising platform for hosting isolated metal atoms. The Ru atom is found to preferentially anchor at the C₄ hollow site, yielding a ΔGH* of -0.093 eV, comparable to H on Pt(111). Furthermore, Two Ru decorated BPN (2Ru-BPN) is energetically stable and provided to be as a double atoms catalyst (DACs). The active sit in 2Ru-BPN can lead to the multi-hydrogen adsorptions with Gibbs free energy change of about -0.12 eV, and thus promote the H₂ evolution along Tafel pathway under thermoneutral condition. Thus, this work provides a theoretical blueprint for designing high-performance Ru-based SACs and reinforces the potential of BPN as a next-generation catalyst support in hydrogen production.

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.