It is highly desired to improve the visible‐light activity of g‐C3N4 for H2 evolution by constructing closely contacted heterojunctions with conductive polymers. Herein, a polymer nanocomposite photocatalyst with high visible‐light activity is fabricated successfully by coupling nanosized polypyrrole (NPPy) particles onto g‐C3N4 nanosheets through a simple wet‐chemical process, and its visible‐light activity is improved further by constructing Mg−O bridges between the NPPy and g‐C3N4. The amount‐optimized bridged nanocomposite displays an approximately ninefold improvement in visible‐light activity compared with g‐C3N4. On the basis of transient‐state surface photovoltage responses, photoluminescence spectra, .OH amount evaluation, and photoelectrochemical curves, it is concluded that the exceptional photoactivity can be attributed to the significantly promoted charge transfer and separation along with visible photosensitization from NPPy. Interestingly, it is confirmed that the promoted charge separation depends mainly on the excited high‐level electron transfer from g‐C3N4 to NPPy by single‐wavelength photocurrent action spectra. This work provides a feasible strategy for designing polymer nano‐heterojunction photocatalysts with exceptional visible‐light activities.
Unraveling the sluggish charge separation, insufficient catalytic
sites, and limited visible-light absorption for Z-scheme heterojunction
photocatalysts still remains a great challenge toward CO2 conversion. Herein, ultrafine Au-modulated copper phthalocyanine/BiVO4 nanosheet heterojunctions (CuPc/Au-BVNS) with wide-visible-light
responses have been successfully fabricated as efficient photocatalysts
for CO2 conversion to CO, achieving 9-time and 35-time
photoactivity improvement compared to pristine BVNS (ca. 5 nm) and
the previously reported BiVO4 nanoflake (ca. 15 nm), respectively.
The exceptional photoactivity is mainly attributed to the ultrafine
Au interfacial modulation, which is well capable of inducing the directional
electron migration of BVNS and the highly dispersed CuPc assembly
with the increased loading amount, synergistically strengthening the
Z-scheme charge transfer and separation mainly based on the surface
photovoltage spectroscopy assisted with the monochromatic beam and
electron paramagnetic resonance technique. Moreover, the in situ diffuse
reflectance infrared Fourier transform spectroscopy, CO2 temperature-programmed desorption measurement, and electrochemical
results demonstrate that the central metal Cu2+ in the
high-dispersion CuPc exhibits potential catalytic functions for CO2 reduction, much superior to other metals in MPc (M = Co and
Ni)-modified ones. This work highlights the importance of strengthening
artificial Z-scheme charge transfer and provides new strategies for
designing BiVO4-based heterojunctions by controllably assembling
MPc toward efficient solar-driven CO2 conversion.
Graphene-modulated ZnPc/BiVO4 Z-scheme heterojunctions for efficient visible-light catalytic CO2 conversion are achieved by increasing the optimized amount of highly dispersed ZnPc.
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