Zian Xu , Jian Zhu , Zheng Shu , Yu Xia , Rouxi Chen , Shaoqing Chen , Yu Wang , Lin Zeng , Jiacheng Wang , Yongqing Cai , Shi Chen , Fuqiang Huang , Hsing-Lin Wang
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引用次数: 0
摘要
高电流密度或长周期催化导致的金属聚集严重影响了基于钌(Ru)的催化剂在氢进化反应(HER)中的稳定性。在此,我们构建了一种磷(P)诱导的 Ru 簇(1.3 nm)与掺杂氮(N)的碳纤维上的相邻 Ru 单原子集成的抗生长策略(RuSA/NP-PNCFs),用于超稳定 HER。RuSA/NP-PNCFs 具有出色的活性(10 mA cm-2 和 1,000 mA cm-2 时分别为 8 mV 和 132 mV)和创纪录的耐久性(600 mA cm-2 时分别为 100,000 次循环和 1,000 小时)。由于 Ru 和 P/N 之间的结合能和轨道相互作用得到了优化,其尺寸变化仅为 0.8 纳米,而且单原子也得到了很好的保留。实验和理论模拟都表明,杂原子 P 不仅能提高 H2O 的解离能力,还能抑制 HER 过程中 Ru 簇和单个原子的聚集。这项工作为设计用于先进电催化剂的稳定金属团簇-单原子体系提供了有效的策略。
Phosphorus-induced anti-growth of ruthenium clusters-single atoms for ultra-stable hydrogen evolution over 100,000 cycles
Metal aggregation, caused by high current density or long-cycling catalysis, severely affects the stability of ruthenium (Ru)-based catalysts toward hydrogen evolution reaction (HER). Herein, we constructed an anti-growth strategy of phosphorus (P)-induced Ru clusters (1.3 nm) integrated with adjacent Ru single atoms on nitrogen (N)-doped carbon fibers (RuSA/NP-PNCFs) for ultra-stable HER. The RuSA/NP-PNCFs exhibit outstanding activity (8 and 132 mV at 10 and 1,000 mA cm−2) and record durability (100,000 cycles and 1,000 h at 600 mA cm−2). Thanks to the optimized binding energy and orbital interaction between Ru and P/N, the size variation is only 0.8 nm, and single atoms are also well preserved. Both experiments and theoretical simulations indicate that the heteroatom P can not only boost the capacity of H2O dissociation but also suppress the aggregation of Ru clusters and single atoms during HER. This work provides an effective strategy for designing stable metal cluster-single-atom systems for advanced electrocatalysts.
期刊介绍:
Joule is a sister journal to Cell that focuses on research, analysis, and ideas related to sustainable energy. It aims to address the global challenge of the need for more sustainable energy solutions. Joule is a forward-looking journal that bridges disciplines and scales of energy research. It connects researchers and analysts working on scientific, technical, economic, policy, and social challenges related to sustainable energy. The journal covers a wide range of energy research, from fundamental laboratory studies on energy conversion and storage to global-level analysis. Joule aims to highlight and amplify the implications, challenges, and opportunities of novel energy research for different groups in the field.