An-Guo Wu, Jie Ding, Lan Zhao, Hong-Ru Li, Liang-Nian He
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引用次数: 0
Abstract
Carbon dioxide is a major greenhouse gas and a safe, abundant, easily accessible, and renewable C1 resource that can be chemically converted into high value-added chemicals, fuels and materials. The preparation of urea, organic carbonates, salicylic acid, etc. from CO2 through non-reduction conversion has been used in industrial production, while CO2 reduction transformation has become a research hotspot in recent years due to its involvement in energy storage and product diversification. Designing suitable catalysts to achieve efficient and selective conversion of CO2 is crucial due to its thermodynamic stability and kinetic inertness. From this perspective, the redistribution of charges within CO2 molecules through the interaction of Lewis acid/base or metal complexes with CO2, or the forced transfer of electrons to CO2 through photo- or electrocatalysis, is a commonly used effective way to activate CO2. Based on understanding of the activation/reaction mechanism on a molecular level, we have developed metal complexes, metal salts, inorganic/organic salts, ionic liquids, as well as nitrogen rich and porous materials as efficient catalysts for CO2 reductive conversions. The goal of this personal account is to summarize the catalytic processes of CO2 reductive conversion that have been developed in the past 7 years: 1) For the reductive functionalization of CO2, the major challenge lies in accurately adjusting reaction parameters (such as pressure) to achieve high catalytic efficiency and the product selectivity; 2) For photocatalytic or electrocatalytic reduction of CO2, how to suppress competitive hydrogen evolution reactions and improve catalyst stability are key points that requires continuous attention.
二氧化碳是一种主要的温室气体,也是一种安全、丰富、易获取和可再生的 C1 资源,可以通过化学方法转化为高附加值的化学品、燃料和材料。以二氧化碳为原料,通过非还原转化制备尿素、有机碳酸盐、水杨酸等,已在工业生产中得到应用,而二氧化碳还原转化由于涉及能源储存和产品多样化,近年来已成为研究热点。由于二氧化碳的热力学稳定性和动力学惰性,设计合适的催化剂实现二氧化碳的高效和选择性转化至关重要。从这个角度来看,通过路易斯酸/碱或金属络合物与 CO2 的相互作用使 CO2 分子内的电荷重新分配,或通过光催化或电催化将电子强制转移到 CO2,是活化 CO2 的常用有效方法。基于对分子水平活化/反应机制的理解,我们开发了金属络合物、金属盐、无机/有机盐、离子液体以及富氮多孔材料,作为二氧化碳还原转化的高效催化剂。本报告旨在总结过去 7 年中开发的二氧化碳还原转化催化过程:1)对于 CO2 的还原官能化,主要挑战在于如何精确调节反应参数(如压力)以实现高催化效率和产物选择性;2)对于 CO2 的光催化或电催化还原,如何抑制竞争性氢进化反应和提高催化剂稳定性是需要持续关注的关键点。
期刊介绍:
The Chemical Record (TCR) is a "highlights" journal publishing timely and critical overviews of new developments at the cutting edge of chemistry of interest to a wide audience of chemists (2013 journal impact factor: 5.577). The scope of published reviews includes all areas related to physical chemistry, analytical chemistry, inorganic chemistry, organic chemistry, polymer chemistry, materials chemistry, bioorganic chemistry, biochemistry, biotechnology and medicinal chemistry as well as interdisciplinary fields.
TCR provides carefully selected highlight papers by leading researchers that introduce the author''s own experimental and theoretical results in a framework designed to establish perspectives with earlier and contemporary work and provide a critical review of the present state of the subject. The articles are intended to present concise evaluations of current trends in chemistry research to help chemists gain useful insights into fields outside their specialization and provide experts with summaries of recent key developments.