We herein demonstrate the unusual effectiveness of two strategies in combination to enhance photoelectrochemical water splitting. First, the work function adjustment via molybdenum (Mo) doping significantly reduces the interfacial energy loss and increases the open-circuit photovoltage of bismuth vanadate (BiVO
4
) photoelectrochemical cells. Second, the creation and optimization of the heterojunction of boron (B) doping carbon nitride (C
3
N
4
) and Mo doping BiVO
4
to enforce directional charge transfer, accomplished by work function adjustment via B doping for C
3
N
4
, substantially boost the charge separation of photo-generated electron-hole pairs at the B-C
3
N
4
and Mo-BiVO
4
interface. The synergy between the above efforts have significantly reduced the onset potential, and enhanced charge separation and optical properties of the BiVO
4
-based photoanode, culminating in achieving a record applied bias photon-to-current efficiency of 2.67% at 0.54 V vs. the reversible hydrogen electrode. This work sheds light on designing and fabricating the semiconductor structures for the next-generation photoelectrodes.
Creatively
constructing Z-scheme composites is a promising and
common strategy for designing effective photocatalyst systems. Herein,
we synthesized Z-scheme Fe2O3@Ag–ZnO@C
heterostructures from the Fe-MOFs and applied it to photodegradation
of tetracycline and methylene blue pollutants in wastewater. The optimized
sample exhibits a remarkable performance as well as stability under
visible light irradiation. The calculating and experimental results
demonstrate that the Fe2O3@ZnO nanointerface
and carbon sheath together boost the transfer efficiency of photogenerated
carriers and absorption ability, thereby improving the photocatalytic
activity. Furthermore, detailed mechanism investigation reveals the
pivotal role of reactive oxygen species (•OH and •O2
–) generated, resulting
in remarkable performance. In addition, cell biology experiments reveal
that the wastewater after photocatalytic treatment has good biological
compatibility, which is important for applications. This work provides
valuable information for constructing high-performance Z-scheme photocatalysts
from MOFs for environmental treatment.
Electrochemical
CO2 reduction (CO2R) powered
by renewable energy to convert CO2 molecules into formate
is of great interest. It is still challenging to develop an efficient
CO2R catalyst with high selectivity. Herein, we adjust
the adsorption states of CO2
– intermediates
to improve the selectivity of CO2 toward formate by doping
S to Cu-based electrocatalysts. It can be found that S doping could
stabilize the reductive-state Cu as the active site for CO2R. The vibration models of CO2
– intermediates
within in situ Raman spectroscopy reveal that the selectivity improvement
is ascribed to the change of the adsorption state from coexisting
O*CO– and OC*O*– to the dominating
OC*O*–. The electrocatalyst manifests high selectivity
and activity toward formate (maximum Faradaic efficiency as high as
76.5% and maximum partial current density 21.06 mA cm–2).
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