Photocatalytic
CO2 conversion to fuels is a promising
strategy for achieving global carbon neutrality. However, infrared
light, which accounts for ∼50% of the full sunlight spectrum,
has not yet been effectively utilized via photocatalysis. Here, we
present an approach to directly power photocatalytic CO2 reduction using near-infrared light. This near-infrared light-responsive
process occurs on an in situ generated Co3O4/Cu2O photocatalyst with a nanobranch structure.
Photoassisted Kelvin probe force microscopy and relative photocatalytic
measurements demonstrate the increase of surface photovoltage after
illumination by near-infrared light. We also find that Cu(I) on this in situ generated Co3O4/Cu2O could facilitate the formation of a *CHO intermediate, thus enabling
a high-performance CH4 production with a yield of 6.5 μmol/h
and a selectivity of 99%. Moreover, we perform a practically oriented
direct solar-driven photocatalytic CO2 reduction under
concentrated sunlight and achieve a fuel yield of 12.5 μmol/h.
Electrochemical
CO2 reduction technology plays an important
role in reducing CO2 into valuable chemical fuels. Therein,
Cu-based catalysts show superior performance for producing high-value
C2+ products. Here, we illustrate the ascendency of high-index
facets of Cu catalysts in producing C2+ products and find
that two kinds of sites favor C–C coupling on the surface.
One is prone to adsorb the C–C coupling structure by spanning
stepped coppers with different coordination numbers. The other is
to embed the structure along two columns of Cu with similar characteristics
through O and C adsorbed simultaneously. Within all research surfaces,
the coupling energy barrier is lowest on the Cu(911) facet, which
is consistent with the experiment. The less charged sites promote
the stabilization of the CO–CO structure as determined by charge
analysis. Furthermore, our results suggest that the high selectivity
for C2+ products on a Cu surface could significantly come
from the contribution of the high-index facet.
Coal consumption leads to over 15 billion tons of global CO2 emissions annually, which will continue at a considerable intensity in the foreseeable future. To remove the huge amount of CO2, a practically feasible way of direct carbon mitigation, instead of capturing that from dilute tail gases, should be developed; as intended, we developed two innovative supporting technologies, of which the status, strengths, applications, and perspective are discussed in this paper. One is supercritical water gasification-based coal/biomass utilization technology, which orderly converts chemical energy of coal and low-grade heat into hydrogen energy, and can achieve poly-generation of steam, heat, hydrogen, power, pure CO2, and minerals. The other one is the renewables-powered CO2 reduction techniques, which uses CO2 as the resource for carbon-based fuel production. When combining the above two technical loops, one can achieve a full resource utilization and zero CO2 emission, making it a practically feasible way for China and global countries to achieve carbon neutrality while creating substantial domestic benefits of economic growth, competitiveness, well-beings, and new industries.
Understanding the synergistic effect of Cu-based alloys on the adsorption behavior and selectivity of the CO 2 reduction reaction is a crucial step toward directional catalyst design. To this end, density functional theory calculations are employed to investigate Cu-based alloys with diverse doping elements and contents. The results show that the scaling relation still holds in the alloy system, and the strategies to improve the selectivity are put forward based on the adsorption strength of *C and *OCHO intermediates. Further, a model combining the adsorption theory and machine learning algorithm is proposed to capture the relationship between the adsorption energy and the geometric environment. It explains that the difference in d-band centers between the doped metals and Cu affects the variation trend of the adsorption strength and reveals that the intermetallic synergistic effect can be quantified by the bonding distance and d orbital radius on both the adsorbate and metal side.
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