Guo Chengyu, Shen Long-Yun, Tang Yujun, Ciucci Francesco, Tang Zhenghua
School of Environment and Energy, Guangzhou Higher Education Mega Center, New Energy Research Institute, South China University of Technology, Guangzhou, China.
Division of Emerging Interdisciplinary Areas, The Hong Kong University of Science and Technology, Clear Water Bay, Hong Kong SAR, P. R. China.
ChemSusChem. 2025 Apr 14;18(8):e202401418. doi: 10.1002/cssc.202401418. Epub 2024 Oct 18.
Electrochemical NO reduction reaction (NORR) represents a green and sustainable way to produce valuable NH for both NH production and nitrate contaminant removal, and developing efficient, durable, highly selective catalyst is the key. Herein, we report a facile method to fabricate a catalyst composed of ultrafine Cu nanowires (Cu NWs) encapsulated by ZIF67, namely, CuNW@ZIF67, for efficient NH electrosynthesis from nitrate. The CuNW@ZIF67 catalyst exhibited excellent catalytic performance toward NORR in alkaline electrolyte, manifested by a large NH Faradaic efficiency of 93.7 % at -0.5 V versus reversible hydrogen electrode (RHE), a high energy efficiency over 30 % at -0.7 V, and robust long-term stability. Such intriguing catalytic properties are mainly ascribed to its structural merits and the strong electronic interaction between Cu NWs and ZIF67. DFT calculations revealed that, the Cu site can easily convert NO into NO , while the Co site plays a critical role in catalyzing the NO -to-NH process. The study can shed light on rational design of efficient, durable, and highly selective catalysts for NORR and beyond.
电化学NO还原反应（NORR）是一种绿色可持续的方法，可用于生产有价值的NH₃，既可以用于合成氨，也可以用于去除硝酸盐污染物，而开发高效、耐用、高选择性的催化剂是关键。在此，我们报道了一种简便的方法来制备一种由ZIF67包裹的超细铜纳米线（Cu NWs）组成的催化剂，即CuNW@ZIF67，用于从硝酸盐中高效电合成NH₃。CuNW@ZIF67催化剂在碱性电解质中对NORR表现出优异的催化性能，在相对于可逆氢电极（RHE）为-0.5 V时，NH₃的法拉第效率高达93.7%，在-0.7 V时能量效率超过30%，并且具有强大的长期稳定性。这种引人入胜的催化性能主要归因于其结构优点以及Cu NWs与ZIF67之间强烈的电子相互作用。密度泛函理论（DFT）计算表明，Cu位点可以轻松地将NO转化为NO₂，而Co位点在催化NO₂到NH₃的过程中起关键作用。该研究可为NORR及其他领域高效、耐用、高选择性催化剂的合理设计提供启示。
