Sequential *CO management via controlling in situ reconstruction for efficient industrial-current-density CO2-to-C2+ electroreduction.
Proc Natl Acad Sci U S A
; 120(40): e2302851120, 2023 Oct 03.
Article
in En
| MEDLINE
| ID: mdl-37748076
ABSTRACT
Sequentially managing the coverage and dimerization of *CO on the Cu catalysts is desirable for industrial-current-density CO2 reduction (CO2R) to C2+, which required the multiscale design of the surface atom/architecture. However, the oriented design is colossally difficult and even no longer valid due to unpredictable reconstruction. Here, we leverage the synchronous leaching of ligand molecules to manipulate the seeding-growth process during CO2R reconstruction and construct Cu arrays with favorable (100) facets. The gradient diffusion in the reconstructed array guarantees a higher *CO coverage, which can continuously supply the reactant to match its high-rate consumption for high partial current density for C2+. Sequentially, the lower energy barriers of *CO dimerization on the (100) facets contribute to the high selectivity of C2+. Profiting from this sequential *CO management, the reconstructed Cu array delivers an industrial-relevant FEC2+ of 86.1% and an FEC2H4 of 60.8% at 700 mA cm-2. Profoundly, the atomic-molecular scale delineation for the evolution of catalysts and reaction intermediates during CO2R can undoubtedly facilitate various electrocatalytic reactions.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
Proc Natl Acad Sci U S A
Year:
2023
Type:
Article