Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 19, Pages 7402-7413Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00946
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Funding
- National Natural Science Foundation of China [21972015, 22088102]
- Young top talents project of Liaoning Province [XLYC1907147]
- Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science [2019JH3/30100003]
- Fundamental Research Funds for the Central Universities [DUT20TD06]
- Swedish Research Council
- K&A Wallenberg Foundation
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By utilizing a three-dimensional ordered macroporous inverse opal array and an ultrathin carbon-nitride-based layer intercalated technology, significant improvements were achieved in the performance of photoelectrochemical water splitting. The conformal heterojunction photoanode exhibited high current density and incident photon-to-current efficiency under simulated sunlight illumination, showcasing a promising approach for sustainable energy conversion systems.
Direct photoelectrochemical (PEC) water splitting is of prime importance in sustainable energy conversion systems; however, it is a big challenge to simultaneously control light harvesting and charge transport for the improvement of PEC performance. Herein, we report a three-dimensional ordered macroporous (3DOM) CsTaWO6-xNx inverse opal array as a promising candidate for the first time. To address the critical challenge, an ultrathin carbon-nitride-based layer-intercalated 3DOM CsTaWO6-xNx architecture as a conformal heterojunction photoanode was assembled. This state-of-the-art conformal heterojunction photoanode with carrier-separation efficiency up to 88% achieves a high current density of 4.59 mA cm(-2) at 1.6 V versus a reversible hydrogen electrode (vs RHE) under simulated AM 1.5G illumination, which is approximately 3.4 and 17 times larger than that of pristine CsTaWO6-xNx inverse opals and powers photoelectrodes in alkaline media, corresponding to an incident photon-to-current efficiency of 32% at 400 nm and outstanding stability for PEC water splitting. Density functional theory calculations propose that the intimate interface of a conformal photoanode optimizes the charge separation and transfer, thus enhancing the intrinsic water oxidation performance. This work enables us to elucidate the pivotal importance of 3DOM architectures and conformal heterostructures and the promising contributions to excellent PEC water-splitting applications.
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