Integrating CO<sub>2</sub> electroreduction with phenol hydrogenation on an oxygen-affinity tailored catalyst.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40880487.
- Also identified by DOI 10.1126/sciadv.ady4981 and PMC identifier 12396342.
- Licence recorded as CC BY-NC.
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Abstract
Electrocatalytic CO<sub>2</sub> reduction (ECR) to formic acid faces challenges in separating and purifying a formate-electrolyte mixture. In situ utilization of this mixture presents a promising yet underexplored solution. Here, we report the synthesis of Bi<i><sub>x</sub></i>Pd<sub>1-</sub><i><sub>x</sub></i>Te nanocrystals (NCs) via a microwave-assisted cation topological exchange approach, enabling the precise tuning of surface oxygen affinities to simultaneously optimize the ECR and catalytic transfer hydrogenation (CTH) of phenol. Optimized Bi<sub>0.1</sub>Pd<sub>0.9</sub>Te NCs achieve a 92% formate Faradaic efficiency at -0.9 volts versus reversible hydrogen electrode and a production rate of 860 millimoles per hour per gram of catalyst at 100 milliamperes per square centimeter. This formate-electrolyte mixture serves as an effective hydrogen donor, enabling 98% selectivity toward cyclohexanone in phenol hydrogenation. Mechanistic studies show uniformly dispersed Bi sites create an oxygen affinity gradient, enhancing *OCHO adsorption for formate production and promoting noncoplanar phenol adsorption for selective cyclohexanone formation. This work pioneers synergistic ECR-CTH integration, establishing an innovative CO<sub>2</sub> valorization and biomass upgrading strategy.