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Hydrogen-bond catalysis in biomass valorization
Chem ( IF 19.1 ) Pub Date : 2024-12-16 , DOI: 10.1016/j.chempr.2024.11.002 Yingchuan Zhang, George W. Huber, Zhengxiao Guo
Chem ( IF 19.1 ) Pub Date : 2024-12-16 , DOI: 10.1016/j.chempr.2024.11.002 Yingchuan Zhang, George W. Huber, Zhengxiao Guo
As a biomimetic concept of enzymatic catalysis, hydrogen-bond catalysis (HBC) leverages H-bond-inducing atomic sites or functional groups in catalysts to regulate substrate binding and transition states so as to enable highly efficient and (stereo)selective organic reactions. However, it has rarely been employed in catalytic biomass valorization toward renewable fuels and value-added chemicals until recently. This perspective aims to highlight the opportunities offered by HBC to promote effective transformations of biomass-derived oxygenates. The concept and characterization approaches of HBC strategies are first introduced, followed by a critical overview of HBC-involved reactions, catalyst structures, and dynamic interfaces between biomass substrates and catalysts. Particular attention is paid to binding configurations and adsorption energetics for which engineered H-bonds can tune bond cleavage/formation and promote desirable reaction pathways in association with intrinsic catalytic sites (e.g., Lewis/Brønsted acid sites, metal active sites, and photogenerated charges) and therefore enable biomass valorization in more efficient and sustainable manners.
中文翻译:
生物质增值中的氢键催化
氢键催化 (HBC) 作为酶催化的仿生概念,利用催化剂中的 H 键诱导原子位点或官能团来调节底物结合和过渡态,以实现高效和(立体)选择性有机反应。然而,直到最近,它才很少用于可再生燃料和增值化学品的催化生物质增值。该观点旨在强调 HBC 为促进生物质衍生含氧化合物的有效转化提供的机会。首先介绍了 HBC 策略的概念和表征方法,然后对 HBC 涉及的反应、催化剂结构以及生物质底物和催化剂之间的动态界面进行了批判性概述。特别关注结合构型和吸附能量,其中工程化的 H 键可以调节键裂解/形成,并促进与本征催化位点(例如,Lewis/Brønsted 酸位点、金属活性位点和光生电荷)相关的理想反应途径,从而以更高效和可持续的方式实现生物质增值。
更新日期:2024-12-16
中文翻译:
生物质增值中的氢键催化
氢键催化 (HBC) 作为酶催化的仿生概念,利用催化剂中的 H 键诱导原子位点或官能团来调节底物结合和过渡态,以实现高效和(立体)选择性有机反应。然而,直到最近,它才很少用于可再生燃料和增值化学品的催化生物质增值。该观点旨在强调 HBC 为促进生物质衍生含氧化合物的有效转化提供的机会。首先介绍了 HBC 策略的概念和表征方法,然后对 HBC 涉及的反应、催化剂结构以及生物质底物和催化剂之间的动态界面进行了批判性概述。特别关注结合构型和吸附能量,其中工程化的 H 键可以调节键裂解/形成,并促进与本征催化位点(例如,Lewis/Brønsted 酸位点、金属活性位点和光生电荷)相关的理想反应途径,从而以更高效和可持续的方式实现生物质增值。