摘要：SummaryPhotoelectrochemical CO2reduction into syngas (a mixture of CO and H2) provides a promising route to mitigate greenhouse gas emissions and store intermittent solar energy into value-added chemicals. Design of photoelectrode with high energy conversion efficiency and controllable syngas composition is of central importance but remains challenging. Herein, we report a decoupling strategy using dual cocatalysts to tackle the challenge based on joint computational and experimental investigations. Density functional theory calculations indicate the optimization of syngas generation using a combination of fundamentally distinctive catalytic sites. Experimentally, by integrating spatially separated dual cocatalysts of a CO-generating catalyst and a H2-generating catalyst with GaN nanowires on planar Si photocathode, we report a record high applied bias photon-to-current efficiency of 1.88% and controllable syngas products with tunable CO/H2ratios (0–10) under one-sun illumination. Moreover, unassisted solar CO2reduction with a solar-to-syngas efficiency of 0.63% is demonstrated in a tandem photoelectrochemical cell.Graphical AbstractDisplay OmittedHighlights•Combined experimental and theoretical investigations were performed•A record high applied bias photon-to-current efficiency of 1.88% was achieved•The CO/H2ratio in the syngas product can be controllably tuned in a wide range•Unassisted syngas generation was proved in a tandem photoelectrochemical cellCatalysis; Electrochemical Energy Conversion; Nanomaterials
