【Frontiers in HaiChuan Chemical Technology】A series of significant advancements made by East China University of Science and Technology in the field of selective control in multiphase catalytic reactions
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Recently, the Catalytic Reaction Engineering team from the School of Chemical Engineering at East China University of Science and Technology was invited by the journal Chemical Reviews of the American Chemical Society to publish online a review article titled “Regulating the Selectivity of Heterogeneous Catalytic Reactions via Configuration-Matching Strategies.” This article provides a comprehensive summary of the selective regulation strategies based on adsorption configuration matching that the team has developed in recent years, as well as the research progress achieved through these strategies in the design of heterogeneous catalysts. Heterogeneous catalysis is of great significance to the chemical industry, being widely applied in areas such as energy conversion, fine chemicals, and environmental protection. Its core objective is to maximize the selectivity of the desired product while efficiently converting the reactants, and to reduce the formation of by-products. Highly selective catalytic technologies can significantly reduce energy consumption and waste emissions; they are not only directly related to production efficiency and cost control, but also play a key role in achieving green and sustainable chemical processes. However, due to the existence of multiple competitive reaction pathways in catalytic reactions, precisely controlling the selectivity of these reactions to achieve directed transformation has long been a challenge in the field of catalysis. Through years of systematic research, the research team has found that the adsorption configuration of the reactants on the catalyst surface is the key factor determining the reaction pathway. Based on this, the team innovatively proposed the design concept of \"adsorption configuration matching\": by precisely regulating the structure and electronic properties of the catalyst’s active sites, it is possible to achieve a targeted fit with the structural characteristics of the substrate molecules, thereby preferentially stabilizing the adsorption pattern required for the desired reaction while suppressing competitive adsorption and side reaction pathways.
Three typical strategies for regulating adsorption configurations: For small molecular unsaturated compounds such as acetylene, the team employed a site-separation strategy to increase the distance between metal atoms on the catalyst surface, thereby disrupting those adsorption configurations involving multi-σ bonds that could lead to excessive hydrogenation. This approach forced the reactants to adsorb through π bonds, achieving high-selective conversion of acetylene into ethylene and effectively suppressing the formation of ethane and C4 by-products. For polyfunctional molecules such as glycerol and dimethyl oxalate, the oxygen-affinity of metal-oxide interfaces is utilized to achieve selective anchoring and activation of specific functional groups in the substrate; simultaneously, hydrogen molecules are also activated, enabling the directed transformation of these polyfunctional molecules in reactions such as the conversion of glycerol into dihydroxy**, and the hydrogenation of dimethyl oxalate to produce methyl glycolate. When dealing with aromatic compounds and cyclic molecules, the confinement effect of nanopores together with the \"geometric gating\" function of the porous coating is utilized to control the adsorption orientation of the reactant molecules, forcing those that would otherwise tend to adsorb in a flat position to adopt an upright adsorption mode. At the same time, the hydrogen diffusion rate can be precisely regulated, thereby enabling selective hydrogenation-deoxygenation or partial hydrogenation reactions. This approach provides new strategies for the purification of fuel oils and the directional transformation of aromatic compounds.
The theoretical basis of the site isolation strategy: The core of the adsorption configuration matching strategy lies in establishing a precise relationship between the characteristics of the catalyst’s active sites, the adsorption configuration of the reactants, and reaction selectivity, thereby enabling a transition from \"empirical design\" to \"precise control\". Through a series of studies, this team demonstrated that catalysts designed based on this principle exhibit excellent selectivity and stability in various key catalytic reactions; these research findings provide new design approaches for the selective control of heterogeneous catalysis. The team also pointed out that this regulatory strategy is not a panacea and requires tailored design based on the reaction system. For example, excessively strong or dense oxygen-loving sites at the metal-oxide interface may lead to the simultaneous activation of multiple groups on polyfunctional substrates, thereby reducing reaction selectivity ； The pore confinement strategy requires precise control of pore size to ensure adsorption orientation selectivity while also maintaining mass transfer efficiency. It is reported that in the future, the team will further develop high-performance catalysts for more reaction processes based on the adsorption configuration matching strategy, thereby promoting the application of catalytic technology in areas such as sustainable energy conversion and waste resource utilization, and contributing to the green and low-carbon transformation of the chemical and energy industries.
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