A rational design of an electrocatalyst presents a promising avenue for solar fuels synthesis from carbon dioxide (CO2) fixation but is extremely challenging. Herein, we use density functional theory calculations to study an inexpensive binary copper−iron catalyst for photoelectrochemical CO2 reduction toward methane. The calculations of reaction energetics suggest that Cu and Fe in the binary system can work in synergy to significantly deform the linear configuration of CO2 and reduce the high energy barrier by stabilizing the reaction intermediates, thus spontaneously favoring CO2 activation and conversion for methane synthesis. Experimentally, the designed CuFe catalyst exhibits a high current density of −38.3 mA⋅cm−2 using industry-ready silicon photoelectrodes with an impressive methane Faradaic efficiency of up to 51%, leading to a distinct turnover frequency of 2,176 h−1 under air mass 1.5 global (AM 1.5G) one-sun illumination.
Large-scale,
clean, efficient, and sustainable hydrogen production
from water is one of the major goals in solar-to-fuel conversion as
the sun and water represent the two most abundant and geographically
balanced free resources available on earth. Considering that most
of the liquid water available on the earth’s surface is present
in the form of seawater, H2 generation from seawater splitting
is highly desirable for large-scale practical and economical application.
Herein, we report on the first demonstration of direct efficient overall
solar-driven seawater splitting on p-GaN-based nanowire
arrays without any external bias or sacrificial agents from various
types of simulated seawater solutions. A stable solar-to-hydrogen
(STH) conversion efficiency of 1.9% was obtained under concentrated
irradiation, demonstrating its possible utilization for the large-scale,
environmentally friendly, sustainable generation of clean solar fuel.
The combination of earth-abundant catalysts and semiconductors, for example, molybdenum sulfides and planar silicon, presents a promising avenue for the large-scale conversion of solar energy to hydrogen. The inferior interface between molybdenum sulfides and planar silicon, however, severely suppresses charge carrier extraction, thus limiting the performance. Here, we demonstrate that defect-free gallium nitride nanowire is ideally used as a linker of planar silicon and molybdenum sulfides to produce a high-quality shell-core heterostructure. Theoretical calculations revealed that the unique electronic interaction and the excellent geometric-matching structure between gallium nitride and molybdenum sulfides enabled an ideal electron-migration channel for high charge carrier extraction efficiency, leading to outstanding performance. A benchmarking current density of 40 ± 1 mA cm−2 at 0 V vs. reversible hydrogen electrode, the highest value ever reported for a planar silicon electrode without noble metals, and a large onset potential of +0.4 V were achieved under standard one-sun illumination.
A unique GaN:Sn nanoarchitecture is integrated on planar silicon to demonstrate an energetically favorable reaction path for aqueous photoelectrochemical CO2 reduction towards formic acid with high efficiency at low overpotential.
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