Liu Haipeng, Wang Peike, Qi Xue, Yin Ao, Wang Yuxin, Ye Yang, Luo Jingjing, Ren Zhongqi, Chen Lina, Yu Suzhu, Wei Jun
Shenzhen Key Laboratory of Flexible Printed Electronics Technology, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China.
School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China.
Molecules. 2024 Jul 15;29(14):3321. doi: 10.3390/molecules29143321.
Nickel-based catalysts are regarded as the most excellent urea oxidation reaction (UOR) catalysts in alkaline media. Whatever kind of nickel-based catalysts is utilized to catalyze UOR, it is widely believed that the in situ-formed Ni moieties are the true active sites and the as-utilized nickel-based catalysts just serve as pre-catalysts. Digging the pre-catalyst effect on the activity of Ni moieties helps to better design nickel-based catalysts. Herein, five different anions of OH, CO, SiO, MoO, and WO were used to bond with Ni to fabricate the pre-catalysts -Ni(OH), Ni-CO, Ni-SiO, Ni-MoO, and Ni-WO. It is found that the true active sites of the five as-fabricated catalysts are the same in situ-formed Ni moieties and the five as-fabricated catalysts demonstrate different UOR activity. Although the as-synthesized five catalysts just serve as the pre-catalysts, they determine the quantity of active sites and activity per active site, thus determining the catalytic activity of the catalysts. Among the five catalysts, the amorphous nickel tungstate exhibits the most superior activity per active site and can catalyze UOR to reach 158.10 mA·cm at 1.6 V, exceeding the majority of catalysts. This work makes for a deeper understanding of the pre-catalyst effect on UOR activity and helps to better design nickel-based UOR catalysts.
镍基催化剂被认为是碱性介质中最优异的尿素氧化反应(UOR)催化剂。无论使用哪种镍基催化剂来催化UOR,人们普遍认为原位形成的Ni部分是真正的活性位点,而所使用的镍基催化剂仅作为预催化剂。深入研究预催化剂对Ni部分活性的影响有助于更好地设计镍基催化剂。在此,使用OH、CO、SiO、MoO和WO这五种不同的阴离子与Ni结合来制备预催化剂——Ni(OH)、Ni-CO、Ni-SiO、Ni-MoO和Ni-WO。研究发现,这五种制备好的催化剂的真正活性位点都是原位形成的相同的Ni部分,且这五种制备好的催化剂表现出不同的UOR活性。尽管合成的这五种催化剂仅作为预催化剂,但它们决定了活性位点的数量以及每个活性位点的活性,从而决定了催化剂的催化活性。在这五种催化剂中,非晶态钨酸镍表现出每个活性位点最优异的活性,在1.6 V时能催化UOR达到158.10 mA·cm,超过了大多数催化剂。这项工作有助于更深入地理解预催化剂对UOR活性的影响,并有助于更好地设计镍基UOR催化剂。