Hou Qiankun, Liu Kang, Al-Maksoud Walid, Huang Yuchang, Ding De, Lei Yongpeng, Zhang Yi, Lin Bin, Zheng Lirong, Liu Min, Basset Jean-Marie, Chen Yin
College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, People's Republic of China.
School of Physics and Electronic, Central South University, Changsha, Hunan 410083, People's Republic of China.
ACS Appl Mater Interfaces. 2023 Apr 5;15(13):16809-16817. doi: 10.1021/acsami.3c01228. Epub 2023 Mar 27.
Nonprecious-metal heterogeneous catalysts with atomically dispersed active sites demonstrated high activity and selectivity in different reactions, and the rational design and large-scale preparation of such catalysts are of great interest but remain a huge challenge. Current approaches usually involve extremely high-temperature and tedious procedures. Here, we demonstrated a straightforward and scalable preparation strategy. In two simple steps, the atomically dispersed Ni electrocatalyst can be synthesized in a tens grams scale with quantitative yield under mild conditions, and the active Ni sites were produced by immobilizing preorganized NiN complex on the substrate surface via organic thermal reactions. This catalyst exhibits excellent catalysis performances in both oxygen evolution and reduction reactions. It also exhibited tunable catalysis activity, high catalysis reproducibility, and high stability. The atomically dispersed NiN sites are tolerant at high Ni concentration, as the random reactions and metal nanoparticle formation that generally occurred at high temperatures were avoided. This strategy illustrated a practical and green method for the industrial manufacture of nonprecious-metal single-site catalysts with a predictable structure.
具有原子分散活性位点的非贵金属多相催化剂在不同反应中表现出高活性和选择性,此类催化剂的合理设计和大规模制备备受关注,但仍然是一个巨大的挑战。目前的方法通常涉及极高的温度和繁琐的程序。在此,我们展示了一种直接且可扩展的制备策略。通过两个简单步骤,可在温和条件下以定量产率合成数十克规模的原子分散镍电催化剂,活性镍位点是通过有机热反应将预组装的NiN络合物固定在基底表面而产生的。该催化剂在析氧反应和氧还原反应中均表现出优异的催化性能。它还表现出可调节的催化活性、高催化重现性和高稳定性。原子分散的NiN位点在高镍浓度下具有耐受性,因为避免了通常在高温下发生的随机反应和金属纳米颗粒的形成。该策略为工业制造具有可预测结构的非贵金属单原子催化剂提供了一种实用且绿色的方法。