Wang, B. et al. Heat diffusion-induced gradient energy level in multishell bisulfides for highly efficient photocatalytic hydrogen production. Adv. Energy Mater. 10, 2001575 (2020).

Bajorowicz, B., Nadolna, J., Lisowski, W., Klimczuk, T. & Zaleska-Medynska, A. The effects of bifunctional linker and reflux time on the surface properties and photocatalytic activity of CdTe quantum dots decorated KTaO3 composite photocatalysts. Appl. Catal. B 203, 452–464 (2017).

Jiang, Z. et al. A hierarchical Z‑scheme α-Fe2O3/g-C3N4 hybrid for enhanced photocatalytic CO2 reduction. Adv. Mater. 30, 1706108 (2018).

Li, H. et al. New reaction pathway induced by plasmon for selective benzyl alcohol oxidation on BiOCl possessing oxygen vacancies. J. Am. Chem. Soc. 139, 3513–3521 (2017).

Liu, J. et al. Metal-free efficient photocatalyst for stable visible water splitting via a two-electron pathway. Science 347, 970–974 (2015).

Hirai, H. et al. Doping-mediated energy-level engineering of M@Au12 superatoms (M = Pd, Pt, Rh, Ir) for efficient photoluminescence and photocatalysis. Angew. Chem. Int. Ed. 61, e202207290 (2022).

Ling, C. et al. Atomic-layered Cu5 nanoclusters on FeS2 with dual catalytic sites for efficient and selective H2O2 activation. Angew. Chem. Int. Ed. 61, e202200670 (2022).

Internalquantum efficiency

Liu, F. et al. Direct Z-scheme hetero-phase junction of black/red phosphorus for photocatalytic water splitting. Angew. Chem. Int. Ed. 58, 11791–11795 (2019).

Han, T. et al. Anion-exchange-mediated internal electric field for boosting photogenerated carrier separation and utilization. Nat. Commun. 12, 4952 (2021).

Spectral response

Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou, China

Zhang, W. et al. High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2. Nat. Commun. 13, 2806 (2022).

Wang, L., Zheng, X., Chen, L., Xiong, Y. & Xu, H. van der Waals heterostructures comprised of ultrathin polymer nanosheets for efficient Z-scheme overall water splitting. Angew. Chem. Int. Ed. 57, 3454–3458 (2018).

Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).

Yan, Y. et al. Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%. Nat. Energy 2, 17052 (2017).

量子效率

Oshima, T. et al. An artificial Z-scheme constructed from dye-sensitized metal oxide nanosheets for visible light-driven overall water splitting. J. Am. Chem. Soc. 142, 8412–8420 (2020).

Pan, Z., Zhang, G. & Wang, X. Polymeric carbon nitride/reduced graphene oxide/Fe2O3: all-solid-state Z-scheme system for photocatalytic overall water splitting. Angew. Chem. Int. Ed. 58, 7102–7106 (2019).

He, Y. et al. 3D hierarchical ZnIn2S4 nanosheets with rich Zn vacancies boosting photocatalytic CO2 reduction. Adv. Funct. Mater. 29, 1905153 (2019).

Photoelectric conversionefficiency

Sukhovatkin, V., Hinds, S., Brzozowski, L. & Sargent, E. H. Colloidal quantum-dot photodetectors exploiting multiexciton generation. Science 324, 1542–1544 (2009).

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Wang, Q. et al. Scalable water splitting on particulate photocatalyst sheets with a solar-to-hydrogen energy conversion efficiency exceeding 1%. Nat. Mater. 15, 611–615 (2016).

Li, C. et al. Surviving high-temperature calcination: ZrO2-induced hematite nanotubes for photoelectrochemical water oxidation. Angew. Chem. Int. Ed. 56, 4150–4155 (2017).

Sun, X. et al. Enhanced superoxide generation on defective surfaces for selective photooxidation. J. Am. Chem. Soc. 141, 3797 (2019).

Sun, S. et al. Engineering interfacial band bending over bismuth vanadate/carbon nitride by work function regulation for efficient solar-driven water splitting. Sci. Bull. 67, 389–397 (2022).

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Semonin, O. E. et al. Peak external photocurrent quantum efficiency exceeding 100% via MEG in a quantum dot solar Cell. Science 334, 1530–1533 (2011).

Wang, J. et al. Porphyrin conjugated polymer grafted onto BiVO4 nanosheets for efficient Z-scheme overall water splitting via cascade charge transfer and single-atom catalytic sites. Adv. Energy Mater. 11, 2003575 (2021).

Chao, Y. et al. Ultrathin visible-light-driven Mo incorporating In2O3–ZnIn2Se4 Z-scheme nanosheet photocatalysts. Adv. Mater. 31, 1807226 (2019).

Zhang, Z., Nagashima, H. & Tachikawa, T. Ultra-narrow depletion layers in a hematite mesocrystal-based photoanode for boosting multihole water oxidation. Angew. Chem. Int. Ed. 59, 9047–9054 (2020).

Sun, S. et al. Efficient redox-mediator-free Z-scheme water splitting employing oxysulfide photocatalysts under visible light. ACS Catal. 8, 1690–1696 (2018).

X.L. and Y.Z. proposed the experimental concepts, designed the experiments and prepared the paper. X.L. supervised the project. Y.Z., X.X., Y.W., P.G., R.W. and B.W. carried out the experiments and conducted the materials characterization. W.H. and A.J.S. revised the paper. Y.L. finished the computation. All authors discussed the results and approved the final version of the paper.

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Chen, X., Wang, J., Chai, Y., Zhang, Z. & Zhu, Y. Efficient photocatalytic overall water splitting induced by the giant internal electric field of a g-C3N4/rGO/PDIP Z-scheme heterojunction. Adv. Mater. 33, 2007479 (2021).

Chen, Y. et al. Multiple exciton generation in tin–lead halide perovskite nanocrystals for photocurrent quantum efficiency enhancement. Nat. Photon. 16, 485–490 (2022).

Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).

Ye, Z., Li, T., Ma, G., Dong, Y. & Zhou, X. Metal-ion (Fe, V, Co, and Ni)-doped MnO2 ultrathin nanosheets supported on carbon fiber paper for the oxygen evolution reaction. Adv. Funct. Mater. 27, 1704083 (2017).

quantumefficiency中文

Zhao, D. et al. Boron-doped nitrogen-deficient carbon nitride-based Z-scheme heterostructures for photocatalytic overall water splitting. Nat. Energy 6, 388–397 (2021).

Zhang, P. et al. Photogenerated electron transfer process in heterojunctions: in situ irradiation XPS. Small Methods 4, 2000214 (2020).

Liu, X. et al. Activating the electrocatalysis of MoS2 basal plane for hydrogen evolution via atomic defect configurations. Small 18, e2200601 (2022).

Low, J., Dai, B., Tong, T., Jiang, C. & Yu, J. In situ irradiated X-ray photoelectron spectroscopy investigation on a direct Z-scheme TiO2/CdS composite film photocatalyst. Adv. Mater. 31, 1802981 (2019).

Zhang, Y., Li, Y., Xin, X. et al. Internal quantum efficiency higher than 100% achieved by combining doping and quantum effects for photocatalytic overall water splitting. Nat Energy 8, 504–514 (2023). https://doi.org/10.1038/s41560-023-01242-7

Kroupa, D. M. et al. Enhanced multiple exciton generation in PbS|CdS Janus-like heterostructured nanocrystals. ACS Nano 12, 10084–10094 (2018).

Luo, L. et al. Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light. Nat. Commun. 13, 2930 (2022).

All data generated in this study are provided in the article, its Supplementary Information and the Source data provided with this paper.

Lei, F. et al. Atomic-layer-confined doping for atomic-level insights into visible-light water splitting. Angew. Chem. Int. Ed. 54, 9266–9270 (2015).

Jiang, W. et al. Tuning the anisotropic facet of lead chromate photocatalysts to promote spatial charge separation. Angew. Chem. Int. Ed. 61, e202207161 (2022).

Qi, Y. et al. Redox-based visible-light-driven Z-scheme overall water splitting with apparent quantum efficiency exceeding 10%. Joule 2, 2393–2402 (2018).

Externalquantum efficiency

Materials Research Institute, School of Engineering and Materials Science, Faculty of Science and Engineering, Queen Mary University of London, London, UK

Wang, Y. et al. Sulfur-deficient ZnIn2S4/oxygen-deficient WO3 hybrids with carbon layer bridges as a novel photothermal/photocatalytic integrated system for Z-scheme overall water splitting. Adv. Energy Mater. 11, 2102452 (2021).

Department of Chemistry and Centre for Scientific Modeling and Computation, Chinese University of Hong Kong, Hong Kong, China

Solar panelefficiency

Wang, Z. et al. Overall water splitting by Ta3N5 nanorod single crystals grown on the edges of KTaO3 particles. Nat. Catal. 1, 756–763 (2018).

Mak, J. S. W., Farah, A. A., Chen, F. & Helmy, A. S. Photonic crystal fiber for efficient raman scattering of CdTe quantum dots in aqueous solution. ACS Nano 5, 3823–3830 (2011).

Chen, X. et al. Three-dimensional porous g-C3N4 for highly efficient photocatalytic overall water splitting. Nano Energy 59, 644–650 (2019).

Li, J., Cai, L., Shang, J., Yu, Y. & Zhang, L. Giant enhancement of internal electric field boosting bulk charge separation for photocatalysis. Adv. Mater. 28, 4059–4064 (2016).

Multiple exciton generation (MEG), where two or more electron–hole pairs are produced from the absorption of one high-energy photon, could increase the efficiency of light absorbing devices. However, demonstrations of the effect are still scarce in photocatalytic hydrogen production. Moreover, many photocatalytic systems for overall water splitting suffer from poor charge carrier separation. Here we show that a CdTe quantum dot/vanadium-doped indium sulphide (CdTe/V-In2S3) photocatalyst has a built-in electric field and cascade energy band structure sufficient to effectively extract excitons and separate carriers, allowing MEG to be exploited for hydrogen production. We achieve a tunable energy band structure through quantum effects in CdTe and doping engineering of V-In2S3, which induces a 14-fold enhancement in the CdTe/V-In2S3 interfacial built-in electric field intensity relative to pristine CdTe/V-In2S3. We report an internal quantum efficiency of 114% at 350 nm for photocatalytic hydrogen production, demonstrating the utilization of MEG effects. The solar-to-hydrogen efficiency is 1.31%.

Song, X. et al. Overall photocatalytic water splitting by an organolead iodide crystalline material. Nat. Catal. 3, 1027–1033 (2020).

State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an, China

Detectivequantum efficiency

This research is supported by the National Natural Science Foundation of China (22261142666, 52172237), the Shaanxi Science Fund for Distinguished Young Scholars (2022JC-21), the Research Fund of the State Key Laboratory of Solidification Processing (NPU), China (grant no. 2021-QZ-02) and the Fundamental Research Funds for the Central Universities (3102019JC005, D5000220033). All funds were awarded to X.L. We thank the members of the Analytical and Testing Center of Northwestern Polytechnical University for help with X-ray diffraction, XPS and SEM characterization.

Grimme, S., Ehrlich, S. & Goerigk, L. Effect of the damping function in dispersion corrected density functional theory. J. Comput. Chem. 32, 1456–1465 (2011).

Shi, X. et al. Highly selective photocatalytic CO2 methanation with water vapor on single-atom platinum-decorated defective carbon nitride. Angew. Chem. Int. Ed. 61, e202203063 (2022).

Neugebauer, J. & Scheffler, M. Adsorbate–substrate and adsorbate–adsorbate interactions of Na and K adlayers on Al(111). Phys. Rev. B 46, 16067–16080 (1992).

Li, B. et al. In situ monitoring charge transfer on topotactic epitaxial heterointerface for tetracycline degradation at the single-particle level. ACS Catal. 12, 9114–9124 (2022).

Sambur, J. B., Novet, T. & Parkinson, B. A. Multiple exciton collection in a sensitized photovoltaic system. Science 330, 63–66 (2010).