Yang Liu, Liu Huibing, Li Ying, Zhong Lisong, Jin Zhaohui, Xu Xiaopei, Cao Dapeng, Chen Zhongwei
State Key Laboratory of Catalysis, Power Battery & Systems Research Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, China.
Angew Chem Int Ed Engl. 2025 Jan 10;64(2):e202414518. doi: 10.1002/anie.202414518. Epub 2024 Nov 16.
Developing efficient and earth-abundant alkaline HER electrocatalysts is pivotal for sustainable energy, but co-regulating its intricate multi-step process, encompassing water dissociation, OH desorption, and hydrogen generation, is still a great challenge. Herein, we tackle these obstacles by fabricating a vertically integrated electrode featuring a nanosheet array with prominent dual-nitride metallic heterostructures characterized by impeccable lattice matching and excellent conductivity, functioning as a multi-purpose catalyst to fine-tune the bonding affinity with alkaline HER intermediates. Detailed structural characterization and theoretical calculation elucidate that charge redistribution at the heterointerface reduces the O p-W d and H s-W d interactions vs. single nitride, thereby enhancing OH transfer and H release. As anticipated, the resulting WN-NiN/CFP catalyst demonstrates a gratifying low overpotential of 36.8 mV at 10 mA/cm for alkaline HER, while concurrently maintaining operational stability for 1300 h at 100 mA/cm for overall water splitting. This work presents an effective approach to meticulously optimize multiple site-intermediate interactions in alkaline HER, laying the foundation for efficient energy conversion.
开发高效且储量丰富的碱性析氢电催化剂对于可持续能源至关重要，但共同调控其复杂的多步过程，包括水离解、OH脱附和氢气生成，仍然是一项巨大挑战。在此，我们通过制造一种垂直集成电极来克服这些障碍，该电极具有纳米片阵列，其具有显著的双氮化物金属异质结构，其特征在于完美的晶格匹配和优异的导电性，作为一种多功能催化剂来微调与碱性析氢中间体的键合亲和力。详细的结构表征和理论计算表明，与单氮化物相比，异质界面处的电荷重新分布降低了O p-W d和H s-W d相互作用，从而增强了OH转移和H释放。正如预期的那样，所得的WN-NiN/CFP催化剂在碱性析氢反应中，在10 mA/cm²时表现出令人满意的36.8 mV的低过电位，同时在100 mA/cm²下进行全水分解时能保持1300小时的操作稳定性。这项工作提出了一种有效方法来精心优化碱性析氢反应中多个位点-中间体相互作用，为高效能量转换奠定了基础。
