Dynamic evolution in stage-evolving Pd catalysis: unlocking efficient and selective hydrogenation of lignin-derived aldehydes
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ID: 316502
2026
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Abstract
Abstract Selective hydrogenation of lignin-derived aldehydes, particularly achieving high catalyst atomic efficiency under ambient conditions, remains challenging. Here, we developed a stage-evolving Pd catalysis that bridges the functions of distinct Pd states to address this limitation. Operando monitoring reveals a sequential transformation from homogeneous Pd2+ to graphene-confined Pd nanoparticles (~3.26 nm), with each stage making a specific contribution. In the vanillin hydrogenation at 30 °C, this system achieves 99.4% conversion within 30 min with 95.0% yield toward 2-methoxy-4-methylphenol and a remarkable turnover frequency of 673.9 h−1, outperforming conventional static sites Pd catalysts reduced by H2 or NaBH4 (≤42.5% conversion, 12.1% yield). Comprehensive in-situ spectroscopic characterizations, combined with kinetic and theoretical investigations, have elucidated the interfacial reaction pathways governing vanillin hydrogenation at distinct Pd active sites and established the correlation between multi-stage catalysis and product selectivity. Mechanistically, the initial Pd2+ phase facilitates C = O adsorption and subsequent hydrogenation to C-OH (47.47 kJ/mol), whereas the in-situ generated Pd/Graphene promotes H2 homolytic dissociation into H* (rather than hydrogen transfer from the isopropanol solvent) and drives the rate-determining hydrodeoxygenation of C-OH (52.44 kJ/mol). This work paves the way for the rational design of dynamic catalytic systems to achieve atomically efficient hydrogenation of lignin-derived aldehydes.
| Reference Key |
openalex_W7164002691
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| Authors | J Gao, Yang Cao, Yong Guo, Liyang Shi, Jingge Shang, Yun Zhao, Gang Luo, Jiajun Fan, James H Clark, Haifang Mao, Shicheng Zhang |
| Journal | national science review |
| Year | 2026 |
| DOI |
10.1093/nsr/nwag338
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| URL | |
| Keywords | Keywords not found |
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