Reductive amination of biomass aldehydes is a vital process to synthesize chemical intermediates primary amine, but the selectivity is severely compromised by the self-condensation of highly reactive imine intermediates. Herein, we proposed a solution by manipulating the adsorption configuration of secondary imine via defect engineering. Specifically, a gradient reduction strategy was used to adjust the driving force of NiCo alloy crystallization, thus motivating the formation of metal vacancy clusters. The primary amine selectivity was raised from 70.9% to 95.1% with defect concentration increased from 36.1% to 42.5% on catalysts. In situ fourier transform infrared spectroscopy (FTIR) and density functional theory demonstrated metal vacancy clusters induced remarkable NiCo electron transfer, which strengthened electronic coupling between secondary imine with catalyst, resulting in a flat configuration that was conducive to CN bond breakage to guarantee smooth conversion into primary amines. This catalyst exhibited potential real-life application prospects for its low cost, universality in reductive amination of various aldehydes, and long-life reusability.

中文翻译：

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通过镍钴合金的缺陷工程促进伯胺可再生串联合成

生物质醛的还原胺化是合成化学中间体伯胺的重要过程，但高反应性亚胺中间体的自缩合严重影响了选择性。在此，我们提出了一种通过缺陷工程操纵仲亚胺吸附构型的解决方案。具体来说，采用梯度还原策略来调节NiCo合金结晶的驱动力，从而促进金属空位簇的形成。催化剂上的伯胺选择性从70.9%提高到95.1%，缺陷浓度从36.1%提高到42.5%。原位傅里叶变换红外光谱（FTIR）和密度泛函理论表明，金属空位簇诱导了显着的NiCo电子转移，从而加强了仲亚胺与催化剂之间的电子耦合，形成有利于CN键断裂的平面构型保证顺利转化为伯胺。该催化剂以其低成本、在各种醛的还原胺化反应中的通用性和长寿命的可重复使用性而展现出潜在的实际应用前景。