Establishing built-in electric field within single-atom-anchored hollow architectures for efficient solar-thermal regulation in plastic photoreforming

doi:10.1016/S1872-2067(26)64974-1

Chinese Journal of Catalysis ›› 2026, Vol. 84: 301-313.DOI: 10.1016/S1872-2067(26)64974-1

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Establishing built-in electric field within single-atom-anchored hollow architectures for efficient solar-thermal regulation in plastic photoreforming

Yi-Wen Han^a^,^c^,¹, Run-Yu Liu^d^,¹, Yu-Xin Zhang^d^,^e^,¹, Lei Ye^d, Phuc T. T. Nguyen^a, Tian-Jun Gong^c(), Xue-Bin Lu^d, Yao Fu^c(), Ning Yan^a^,^b()

^a Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117585, Singapore
^b Centre for Hydrogen Innovations, National University of Singapore, 1 Engineering Drive 3, Singapore 117580, Singapore
^c State Key Laboratory of Precision and Intelligent Chemistry, Anhui Province Key Laboratory of Biomass Chemistry, University of Science and Technology of China, Hefei 230026, Anhui, China
^d School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, China
^e Center for Water and Ecology, School of Environment, Tsinghua University, Beijing 100084, China

Received:2025-09-01 Accepted:2025-10-30 Online:2026-05-18 Published:2026-04-16
Contact: *E-mail: gongtj@ustc.edu.cn (T.-J. Gong),
fuyao@ustc.edu.cn (Y. Fu),
ning.yan@nus.edu.sg (N. Yan).
About author:¹Contributed equally to this work.
Author contributions
Y.W.H., R.Y.L., Y.X.Z. contributed equally to this work. N.Y. directed the project and conceived of the idea. N.Y., Y.F., Y.W.H., X.B.L., L.Y. designed the catalyst development, characterization, and mechanism experiments. R.Y.L., Y.X.Z., T.J.G., P.T.T.N. performed the synthesis, characterization, and mechanism experiments. N.Y., Y.W.H., wrote the manuscript draft. All the authors participated in the discussion and improvement of the manuscript.
Supported by:
Singapore Ministry of Education, MOE Tier-2 project(MOE-T2EP10221-0020);Singapore National Research Foundation, NRF Investigatorship(NRFI07-2021-0006);China Scholarship Council Program(202406340086);National Natural Science Foundation of China(22293011)

Abstract

Abstract:

The strategic engineering of nanostructure architecture and the in-depth understanding of structure-property relationships are pivotal for photocarrier-behavior dependent solar-thermal regulation. We present a general morphology-structure-control strategy for fabricating the isolated metal sites anchored chalcogenide hollow nanoreactors (single-atom metal/chalcogenide HNR, metal includes Pt, Pd, Ru, chalcogenide includes CdS, ZnIn₂S₄, Zn_0.5Cd_0.5S, CdIn₂S₄), they act as photothermal catalysts for plastic photoreforming. This methodology encompasses confinement cavity modulation via templated chalcogenide epitaxial growth and built-in electric field (BIEF) establishment via defect-mediated interface chemical bond construction. As-fabricated heterostructures integrate multilight scattering and directional charge transfer, leveraging hollow architectures and strong BIEF for stimulating the high-concentration carrier generation and driving continuous photocarrier localization and delocalized-electron transportation, thereby enhancing the photocarrier dynamics. Subsequently, photogenerated electron excitation-induced hot electron generation amplifies the photothermal response at atomically dispersed metal sites. Synergistic photothermal catalysis in these nanoreactors promotes complementary adsorption of key intermediates and unlocks low-dissociation-energy pathways of critical chemical bonds, thereby achieving selective transformation of hydroxyl to carbonyl coupled with clean hydrogen production. This work provides a paradigm for manipulating interfacial BIEFs between hollow nanostructure and single-atom sites, elucidating the substantial impact of these tailored architectures on photocarrier dynamics and solar-thermal regulation.

Key words: Single-atom catalysts, Hollow architectures, Built-in electric field, Photocatalysis, Plastic upcycling

Yi-Wen Han, Run-Yu Liu, Yu-Xin Zhang, Lei Ye, Phuc T. T. Nguyen, Tian-Jun Gong, Xue-Bin Lu, Yao Fu, Ning Yan. Establishing built-in electric field within single-atom-anchored hollow architectures for efficient solar-thermal regulation in plastic photoreforming[J]. Chinese Journal of Catalysis, 2026, 84: 301-313.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64974-1

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Figures/Tables 7

Fig. 1. Schematic diagram depicting the synthesis protocol and unique architectural features of single-atom metal/chalcogenide HNR (exemplified by the single-atom Pt/CdS HNR photocatalyst).

Fig. 2. (a) TEM image of CdS HNR. HADDF-STEM image of single-atom Pt/CdS HNR (b) and EDX analysis at A point (c). (d) AC HAADF-STEM image of single-atom Pt/CdS HNR. HAADF-STEM image and elemental mapping of Cd, S, Pt in single-atom Pt/CdS HNR (e), Cd, S, Ru in single-atom Ru/CdS HNR (f), Cd, S, Pd in single-atom Pd/CdS HNR (g), Zn, In, S, Pt in single-Atom Pt/ZnIn2S4 HNR (h), Cd, In, S, Pt in single-atom Pt/ CdIn2S4 HNR (i), Zn, Cd, S, Pt in single-atom Pt/Zn0.5Cd0.5S4 HNR (j). Scale bars: (d) 2 nm; (a,b) 200 nm; (e-j) 200 nm.

Fig. 3. XRD patterns (a), XPS survey spectra (b), BET analysis (c), Raman spectra (d), EPR spectra (e), UV-vis DRS spectra (f) of synthesized CdS-based materials. High-resolution XPS spectra of Pt 4f (g), S 2p (h) and Cd 3d (i) of CdS HNR, single-atom Pt/CdS HNR, and nanoparticle Pt/CdS HNR. (j) Normalized Pt L3-edge XANES. (k) The FT-EXAFS spectra of single-atom Pt/CdS HNR. (l) The EXAFS spectra of Pt L3-edge in R space and k space. (m-o) WTs of Pt foil, PtS2, and single-atom Pt/CdS HNR.

Fig. 4. (a) Photocatalytic performance evaluation over single-atom metal/chalcogenide HNR (metal = Pt, Pd, Ru; chalcogenide = CdS, ZnIn2S4, CdIn2S4, Zn0.5Cd0.5S). (b) Long-term experiment and recycling experiment over single-atom Pt/CdS HNR. (c-j) Photoreforming of real-world PLA and real-world PET plastics by single-atom metal/chalcogenide HNR.

Fig. 5. Electrostatic potential and work function of pristine CdS (a), CdS HNR (b), and Pt (c). The calculated electron density difference of single-atom Pt/pristine CdS (top and side view) (d,e) and single-atom Pt/CdS HNR (top and side view) (f,g). The simulated free-energy diagram of CdS HNR (h) and single-atom Pt/CdS HNR (i) about consecutive dehydrogenation pathway, dehydrogenation-coupling pathway and decarbonization pathway.

Fig. 6. Atomic force microscope images of pristine CdS (a) and single-atom Pt/CdS HNR (d). Surface potential images of pristine CdS (b,c) and single-atom Pt/CdS HNR (e,f). Photo-triggered CPD differences and surface height profiles of pristine CdS (g) and single-atom Pt/CdS HNR (h). (i-k) In-situ irradiated XPS spectra of Pt 4f, S 2p and Cd 3d in single-atom Pt/CdS HNR.

Fig. 7. Steady-state PL spectra (a), time-resolved PL spectra (b), TPC response spectra (c) and EIS Nyquist plots (d) of CdS-based materials. The 2D transient absorption surface plots (e,f) and the decay signals and surface temperature (inside) (h,i) over pristine CdS and single-atom Pt/CdS HNR. SPV response (g), in-situ EPR spectra (j,k), In-situ DRIFTS experiments (l) of pristine CdS and single-atom Pt/CdS HNR.

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Establishing built-in electric field within single-atom-anchored hollow architectures for efficient solar-thermal regulation in plastic photoreforming

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