单原子锚定的中空纳米反应器中构建内建电场以实现高效塑料光热重整

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

催化学报 ›› 2026, Vol. 84: 301-313.DOI: 10.1016/S1872-2067(26)64974-1

单原子锚定的中空纳米反应器中构建内建电场以实现高效塑料光热重整

韩怡雯^a^,^c^,¹, 刘润雨^d^,¹, 张雨昕^d^,^e^,¹, 叶磊^d, Phuc T. T. Nguyen^a, 龚天军^c(), 吕学斌^d, 傅尧^c(), 颜宁^a^,^b()

^a 新加坡国立大学, 化学与生物分子工程系, 新加坡, 新加坡
^b 新加坡国立大学, 氢能源创新中心, 新加坡, 新加坡
^c 中国科学技术大学, 精准智能化学国家重点实验室, 安徽省生物质化学重点实验室, 安徽合肥 230026, 中国
^d 天津大学环境科学与工程学院, 天津 300350, 中国
^e 清华大学环境学院, 水质与水生态研究中心, 北京 100084, 中国

收稿日期:2025-09-01 接受日期:2025-10-30 出版日期:2026-05-18 发布日期:2026-04-16
通讯作者: *电子信箱: gongtj@ustc.edu.cn (龚天军),
fuyao@ustc.edu.cn (傅尧),
ning.yan@nus.edu.sg (颜宁).
作者简介:¹共同第一作者.
基金资助:
新加坡教育部二级项目(MOE-T2EP10221-0020);新加坡国家研究基金会研究员计划(NRFI07-2021-0006);中国国家留学基金管理委员会项目(202406340086);国家自然科学基金(22293011)

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)

摘要/Abstract

摘要：

光催化塑料重整技术可实现高附加值化学品与氢气的联产. 然而, 由于底物活化路径(如R•/RO•途径)差异, 特定产物的选择性调控仍面临挑战. 光催化剂诱导的光热效应可显著增强化学反应的催化选择性与本征活性. 理想的光热效应调控取决于光生载流子生成与传输行为调控技术的创新突破. 当前载流子行为调控仍面临双重制约: 激子生成效率不足, 电荷迁移(本征驱动力/异质界面相互作用)效率不足. 本研究通过在单原子锚定的中空结构中构建内建电场, 调控载流子行为以增强光热效应, 诱导聚乳酸塑料至丙酮酸的高效选择性转化. 这为先进双功能光热催化剂的设计提供了范式, 验证了光重整技术在塑料污染治理与可再生燃料生产中的双重潜力.

本文发展了一种通用的形貌-结构调控策略, 成功构建了单原子金属(Pt, Pd, Ru)锚定的硫属化物(CdS, ZnIn₂S₄, CdIn₂S₄, Zn_0.5Cd_0.5S)中空纳米反应器. 该策略通过模板导向的硫属化物外延生长实现空腔结构调控, 通过缺陷介导的界面化学键构筑引入内建电场, 从而增强光生载流子的生成/迁移动力学, 并诱导分子特异性催化行为. 具体而言: 中空结构通过多重光散射效应实现宽带光子捕获; 内建电场驱动载流子在晶格缺陷位点局域化, 同时离域电子通过界面金属‒硫化学键进行定向传输; 光生电子在局域表面等离子体共振效应驱动下转化为高能热电子, 定向富集于单原子活性位点. 由于内建电场的引入, 高浓度热电子弛豫寿命显著延长, 有效增强了体系的光热效应. 这不仅促进了关键中间体的互补吸附, 更解锁关键化学键的低解离能路径, 触发热力学有利的连续脱氢过程, 从而驱动选择性羟基至羰基转化. 该催化材料实现了分子内脱氢和分子间C-C耦合反应路径的热力学-动力学联合调控与精准分化. 借助时空尺度原位表征技术(X射线吸收光谱、球差校正-高角环形暗场-扫描透射电子显微镜、开尔文探针力显微镜、飞秒瞬态吸收光谱、原位电子顺磁共振、漫反射红外傅里叶变换光谱)和密度泛函理论模拟揭示电荷生成、传输机制, 从而建立电荷传输行为与特定分子催化行为之间的构-效关联.

综上, 该研究揭示了单原子位点与中空结构及界面电场的协同整合机制在实现高效、高选择性塑料光重整过程中展现出应用潜力. 除塑料升级回收之外, 该研究还为开发多功能光催化剂提供了新思路, 有望解决更广泛的太阳能-化学能转化中的选择性调控挑战.

关键词: 单原子催化剂, 中空结构, 内建电场, 光催化, 塑料升级回收

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

韩怡雯, 刘润雨, 张雨昕, 叶磊, Phuc T. T. Nguyen, 龚天军, 吕学斌, 傅尧, 颜宁. 单原子锚定的中空纳米反应器中构建内建电场以实现高效塑料光热重整[J]. 催化学报, 2026, 84: 301-313.

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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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64974-1

https://www.cjcatal.com/CN/Y2026/V84/I5/301

图/表 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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单原子锚定的中空纳米反应器中构建内建电场以实现高效塑料光热重整

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

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