Selective CO2 electrocatalysis at the pseudocapacitive nanoparticle/ordered-ligand interlayer

Autor: Kim, D, Yu, S, Zheng, F, Roh, I, Li, Y, Louisia, S, Qi, Z, Somorjai, GA, Frei, H, Wang, LW, Yang, P
Rok vydání: 2020
Předmět:
Zdroj: Nature Energy, vol 5, iss 12
Popis: Enzymes feature the concerted operation of multiple components around an active site, leading to exquisite catalytic specificity. Realizing such configurations on synthetic catalyst surfaces remains elusive. Here, we report a nanoparticle/ordered-ligand interlayer that contains a multi-component catalytic pocket for high-specificity CO2 electrocatalysis. The nanoparticle/ordered-ligand interlayer comprises a metal nanoparticle surface and a detached layer of ligands in its vicinity. This interlayer possesses unique pseudocapacitive characteristics where desolvated cations are intercalated, creating an active-site configuration that enhances catalytic turnover by two orders and one order of magnitude against a pristine metal surface and nanoparticle with tethered ligands, respectively. The nanoparticle/ordered-ligand interlayer is demonstrated across several metals with up to 99% CO selectivity at marginal overpotentials and onset overpotentials of as low as 27 mV, in aqueous conditions. Furthermore, in a gas-diffusion environment with neutral media, the nanoparticle/ordered-ligand interlayer achieves nearly unit CO selectivity at high current densities (98.1% at 400 mA cm−2).
Databáze: OpenAIRE