Zhu Changyan, Geng Yun, Yao Xiaohui, Zhu Guangshan, Su Zhongmin, Zhang Min
Institute of Functional Material Chemistry, Faculty of Chemistry, National & Local United Engineering Laboratory for Power Batteries, Northeast Normal University, Changchun, 130024, China.
State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun, 130021, China.
Small Methods. 2023 Mar;7(3):e2201331. doi: 10.1002/smtd.202201331. Epub 2023 Jan 31.
The idealized urea electrocatalyst is crucial to boost the CN coupling reaction and simultaneously suppress their isolated reduction process after adsorbing N and CO molecules. Therefore, the dispersed MN -M'N moiety is investigated systematically, including 26 homonuclear and 650 heteronuclear di-metal systems. After, 205 stable systems are selected using lowest-energy principle and ab initio molecular dynamics simulations. According to three possible pathways, NCON, CO, and OCOH to produce urea, a five-step high-throughput screening method for excellent catalytic activity and a five-aspect high-throughput screening strategy for outstanding catalytic selectivity are proposed, respectively. The potential determined steps and the limiting potential through three pathways are identified. The data indicates both CO pathway and OCOH pathway are more competitive at lower Gibbs free energy. Significantly, the most favorite RuN -CoN combination possesses an extremely low limiting potential of -0.80 V for urea production, meanwhile it exists a strong foundation for experimental preparation. This work not only broadens electrocatalytic potentiality of developing di-metals as two active sites, but also provides a feasible high-throughput screening recipe for urea production.
理想化的尿素电催化剂对于促进CN偶联反应并同时抑制吸附N和CO分子后的孤立还原过程至关重要。因此，系统地研究了分散的MN -M'N部分，包括26种同核和650种异核双金属体系。之后，利用最低能量原理和从头算分子动力学模拟选择了205个稳定体系。根据生成尿素的三种可能途径，即NCON、CO和OCOH，分别提出了一种用于筛选具有优异催化活性的五步高通量筛选方法和一种用于筛选具有出色催化选择性的五方面高通量筛选策略。确定了三种途径的潜在决定步骤和极限电位。数据表明，在较低的吉布斯自由能下，CO途径和OCOH途径更具竞争力。值得注意的是，最受欢迎的RuN -CoN组合在尿素生产中具有极低的-0.80 V极限电位，同时为实验制备奠定了坚实基础。这项工作不仅拓宽了将双金属作为两个活性位点开发的电催化潜力，还为尿素生产提供了一种可行的高通量筛选方法。
