Tan Yuan, Yan Lei, Huang Chuanqi, Zhang Wenna, Qi Haifeng, Kang Leilei, Pan Xiaoli, Zhong Yijun, Hu Yong, Ding Yunjie
Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou, Zhejiang, 311231, P. R. China.
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Department of Chemistry, Zhejiang Normal University, Jinhua, Zhejiang, 321004, P. R. China.
Small. 2021 May;17(21):e2100372. doi: 10.1002/smll.202100372. Epub 2021 Apr 17.
Electrocatalysts for efficient production of ammonia from nitrogen reduction reaction (NRR) under ambient conditions are attracted growing interest in recent years, which demonstrate a great potential to replace the Haber-Bosch method which suffers the problems of the huge energy consumption and massive CO production. In this work, a novel electrocatalyst of Au -Cys-M is fabricated for NRR under ambient conditions, with transition metal ions (e.g., Mo , Fe , Co , Ni ) atomically decorated on Au nanoclusters via thiol bridging. The Au -Cys-Mo catalyst exhibits the highest Faradaic efficiency (26.5%) and NH yield (34.5 µg h mg ) in 0.1 m HCl solution. X-ray photoelectron spectroscopy analysis and high angle annular dark field image-scanning transmission electron microscopy characterization reveal that the electronic structure of Mo is optimized by forming the structure of Au-S-Mo and Mo acts as active sites for activating the nitrogen to promote the electrochemical production of ammonia. This work provides a new insight into the precise fabrication of efficient NRR electrocatalysts.
近年来，用于在环境条件下通过氮还原反应（NRR）高效生产氨的电催化剂引起了越来越多的关注，这显示出其巨大的潜力，有望取代存在高能耗和大量一氧化碳产生问题的哈伯-博施法。在这项工作中，制备了一种用于环境条件下NRR的新型电催化剂Au -Cys-M，其中过渡金属离子（如Mo、Fe、Co、Ni）通过硫醇桥接原子级修饰在金纳米团簇上。Au -Cys-Mo催化剂在0.1 m HCl溶液中表现出最高的法拉第效率（26.5%）和NH产量（34.5 µg h mg ）。X射线光电子能谱分析和高角度环形暗场图像扫描透射电子显微镜表征表明，Mo的电子结构通过形成Au-S-Mo结构得到优化，并且Mo作为激活氮以促进氨电化学产生的活性位点。这项工作为高效NRR电催化剂的精确制备提供了新的见解。
