Ruan Pengpeng, Chen Bili, Zhou Qin, Zhang Hansong, Wang Yahao, Liu Kunlong, Zhou Wenting, Qin Ruixuan, Liu Zhi, Fu Gang, Zheng Nanfeng
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, National and Local Joint Engineering Research Center of Preparation Technology of Nanomaterials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China.
Innovation (Camb). 2022 Dec 14;4(1):100362. doi: 10.1016/j.xinn.2022.100362. eCollection 2023 Jan 30.
Precious metal catalysts are the cornerstone of many industrial processes. Replacing precious metal catalysts with earth-abundant metals is one of key challenges for the green and sustainable development of chemical industry. We report in this work a surprisingly effective strategy toward the development of cost-effective, air-stable, and efficient Ni catalysts by simple surface modification with thiols. The as-prepared catalysts exhibit unprecedentedly high activity and selectivity in the reductive amination of aldehydes/ketones. The thiol modification can not only prevent the deep oxidation of Ni surface to endow the catalyst with long shelf life in air but can also allow the reductive amination to proceed via a non-contact mechanism to selectively produce primary amines. The catalytic performance is far superior to that of precious and non-precious metal catalysts reported in the literature. The wide application scope and high catalytic performance of the developed Ni catalysts make them highly promising for the low-cost, green production of high-value amines in chemical industry.
贵金属催化剂是许多工业过程的基石。用储量丰富的金属取代贵金属催化剂是化学工业绿色可持续发展的关键挑战之一。我们在这项工作中报告了一种令人惊讶的有效策略,即通过用硫醇进行简单的表面改性来开发具有成本效益、空气稳定且高效的镍催化剂。所制备的催化剂在醛/酮的还原胺化反应中表现出前所未有的高活性和选择性。硫醇改性不仅可以防止镍表面深度氧化,使催化剂在空气中具有长保质期,还可以使还原胺化反应通过非接触机制进行,以选择性地生产伯胺。其催化性能远远优于文献中报道的贵金属和非贵金属催化剂。所开发的镍催化剂广泛的应用范围和高催化性能使其在化学工业中低成本、绿色生产高价值胺类方面极具前景。