Our team has long-standing research experience in the development of heterogeneous catalytic materials and fixed-bed reaction processes, with a solid experimental foundation. The main research work in recent years includes:
1. Controlled synthesis of hydrogenation catalysts:
To address the issue of limited selectivity towards aromatic amines when catalytic hydrogenation of multi-substituted nitrobenzenes is performed using noble metal catalysts such as Pd, Pt, and Ru, we designed a strategy to control the adsorption configuration of reactant molecules on nanoparticles to enhance selectivity (Angew. Chem. Int. Ed. 2017, 56, 9747).
Using a template-free seeding method, a series of Pd, Pt, and Ru nanoscale catalysts encapsulated in Beta and MOR zeolites (Pd@Beta, Pd@MOR, Pt@Beta, Pt@MOR, Ru@Beta, Ru@MOR) were prepared. This involved adding metal nanoparticle-containing zeolite seeds into gel precursors for Beta zeolite synthesis, followed by homogeneous mixing and precise control of crystallization time and temperature, to obtain the corresponding zeolite-encapsulated metal nanocatalysts.
Due to the pore size constraints of zeolites, substrate molecules diffuse into the pores and adsorb onto the metal nanoparticles in an upright orientation. Compared to other groups, zeolite-encapsulated metal nanocatalysts exhibit a preferential adsorption of nitro groups, ensuring selective hydrogenation of nitro groups and resulting in aromatic amines with selectivity greater than 90%.
Building upon this work, the applicant extended the synthesis methods for zeolite-based core-shell catalytic materials, successfully preparing zeolite-encapsulated metal nanocatalysts via seed and secondary crystallization methods. These include Beta, MOR, Silicalite-1, and CHA zeolites, loaded with Pt, Pd, Rh, and Ag nanoparticles (Nat. Catal. 2018, 1, 540; Ind. Eng. Chem. Res. 2019, 58, 15453; Acta Phys.-Chim. Sin. 2020, 36, 1912001). These catalysts demonstrated excellent stability in a series of high-temperature reactions, such as water-gas shift, methane oxidation reforming, CO₂ hydrogenation, and high-temperature carbon monoxide oxidation.
2. Directional transformation of biomass resources:
To address the issue of low selectivity in the reaction converting lactic acid diesters to propylene glycol, the applicant successfully synthesized a fully silica-coated mesoporous Beta catalyst (Al-Beta-meso@Si-Beta) via a solid-state synthesis method (Chem. Eng. J. 2024, 479, 147803). The silica shell effectively covers the acidic sites on the surface of conventional Beta zeolite, suppressing the formation of high-molecular-weight reaction intermediates and consequently reducing carbon deposition. As a result, Al-Beta-meso@Si-Beta achieved a significantly higher yield of L-propylene glycol (73.3%) compared to mesoporous Beta (55.7%).
Meanwhile, to overcome the problem of poor selectivity caused by excessive oxidation in the traditional oxidative conversion of lactic esters to pyruvate esters, a direct dehydrogenation process of lactic esters to pyruvate esters was proposed. A copper catalyst rich in positive Cu species supported on oxidized silica was developed, which realized a 91% selectivity for pyruvate ester during direct dehydrogenation of lactic esters (Appl. Catal. B-Environ. 2023, 325, 122329). Theoretical calculations and kinetic studies indicate that the abundant Cu^0–Cu^+ interfaces synergistically catalyze the cleavage of C–H and O–H bonds, being the rate-determining step of the reaction.
Additionally, to address the low product selectivity of traditional catalytic materials in the dehydration of lactic esters to acrylic esters, cations were introduced into Al-rich Beta zeolites via ion-exchange methods. This appropriately increased pore resistance, suppressed carbon buildup, accelerated the main reaction rate, and ultimately achieved a significantly higher acrylic ester yield (87.4%) compared to conventional catalysts (ACS Sustainable Chem. Eng. 2023, 11, 8624).
3. Selective preparation of bio-based diols:
To overcome the bottleneck of low 1,5-pentanediol selectivity in the hydrogenation of furfural using cobalt-based catalysts, the applicant innovatively employed rapid carbon thermal shock synthesis to prepare porous cobalt-cerium composite oxide catalysts rich in divalent Co species and oxygen vacancies. By systematically exploring the relationship between synthesis conditions and the catalysts’ geometric/electronic structures, the mechanism of the synergistic effect between Co^2+ species and oxygen vacancies was elucidated. Experiments demonstrated that this catalyst could effectively regulate the stereochemistry of furfuryl alcohol intermediates, preferentially promoting the dehydrogenation cleavage of the C2–O1 bond in the furan ring. This significantly improved the 1,5-pentanediol selectivity from below 50% with traditional cobalt catalysts to nearly 60%, while maintaining excellent stability in cycle tests (ACS Catal. 2025, under review).
Addressing the core issue of low glycerol conversion to 1,2-propanediol during hydrogenation, the study achieved targeted optimization of metal-support interactions and the distribution of Brønsted/Lewis acid sites by precisely adjusting surface functional groups. Combined with kinetic studies, this clarified the mechanism of cooperative catalysis between solid acid sites and metal sites in C–O bond hydrogenolysis, significantly enhancing glycerol synthesis efficiency (Appl. Catal. B-Environ. 2025, 360, 124524; Biomass & Bioenergy 2023, 174, 106818; see Figure 7). To further enhance the catalyst’s ability to activate hydrogen, an innovative interface structure between metal and titanium oxide nanowires was designed. This structure improved hydrogen adsorption and dissociation performance, approximately doubling the C–O hydrogenolysis rate compared to conventional metal/TiO₂ systems, providing a new strategy for efficient production of biomass-derived polyols (RSC Sustain. 2024, 2, 153; Chem. Commun. 2022, 58, 12349).
