Controlled incorporation of Zn into nitrogen-doped porous carbon boosts the alcohol dehydrogenation to carboxylic acids

Abstract

The dehydrogenation of primary alcohols to carboxylic acids is a crucial process in chemical industries such as fibers and plastics. Carboxylic acids, the resulting products, are not only important chemical raw materials but also fundamental pharmaceutical intermediates. Zn-based catalysts have gained attention as a promising option for this transformation owing to their economic cost and abundant reserves. However, stability issues, including structure collapse and morphological changes, have plagued the reported Zn-based catalysts during this transformation. In response to these challenges, this study focused on the design and development of Zn-based catalysts via controlled incorporation of Zn into nitrogen-doped porous carbon to modulate the numbers of defects and Lewis acid-base site pairs. Through extensive screening of various parameters, the best-performing catalyst, namely Zn@NC-800, exhibited high activity and remarkable stability, surpassing all the reported Zn-based catalysts. Moreover, this catalyst demonstrated great recyclability since it could maintain approximately 90 % yields after 9 cycles. Notably, the product formation rate of this catalyst could reach 3833 μmol·g·h, exceeding that of most reported non-noble metal heterogeneous catalysts. Consequently, this study offers a promising approach for efficiently and stably catalyzing alcohol dehydrogenation reactions using non-noble metals.