中空纳米材料的构建原理及其在光催化制氢和二氧化碳还原反应中的应用

doi:10.1016/S1872-2067(21)63863-9

催化学报 ›› 2022, Vol. 43 ›› Issue (3): 679-707.DOI: 10.1016/S1872-2067(21)63863-9

中空纳米材料的构建原理及其在光催化制氢和二氧化碳还原反应中的应用

李旭力^a^,^b, 李宁^a^,^b, 高旸钦^a^,^b, 戈磊^a^,^b^,^*()

^a中国石油大学(北京)重质油国家重点实验室, 新能源与材料学院, 北京 102249
^b中国石油大学(北京)新能源与材料学院, 材料科学与工程系, 北京 102249

收稿日期:2021-04-20 修回日期:2021-04-20 出版日期:2022-03-18 发布日期:2022-02-18
通讯作者: 戈磊
基金资助:
国家重点研发项目(2019YFC1907602);国家自然科学基金(51572295);国家自然科学基金(21273285);国家自然科学基金(21003157)

Design and applications of hollow-structured nanomaterials for photocatalytic H₂ evolution and CO₂ reduction

Xuli Li^a^,^b, Ning Li^a^,^b, Yangqin Gao^a^,^b, Lei Ge^a^,^b^,^*()

^aState Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum Beijing, Beijing 102249, China
^bDepartment of Materials Science and Engineering, College of New Energy and Materials, China University of Petroleum Beijing, Beijing 102249, China

Received:2021-04-20 Revised:2021-04-20 Online:2022-03-18 Published:2022-02-18
Contact: Lei Ge
Supported by:
National Key R&D Program of China(2019YFC1907602);National Natural Science Foundation of China(51572295);National Natural Science Foundation of China(21273285);National Natural Science Foundation of China(21003157)

摘要/Abstract

摘要：

随着全球经济的快速发展, 能源短缺与环境污染成为当今世界共同关注的热点问题, 开发和利用洁净能源成为当务之急. 近年, 以半导体为基础的光催化技术引起了国内外的广泛关注, 其中包括光催化分解水制氢、光催化还原CO₂、光催化固氮以及光催化降解污染物等. 尤其太阳能驱动的光催化分解水和光催化CO₂还原均可将太阳能转化为可储存和运输的化学能源. 因此, 设计高效稳定的光催化材料具有重要意义. 中空结构材料由于具有比表面积大、光吸收效率高以及载流子传输路径缩短等优点, 在能量转换领域备受关注, 且中空材料的内外表面结构为其它组分的沉积提供了良好的平台. 近年来, 研究人员设计和合成了大量的多级纳米中空复合材料.
本文首先综述了中空材料的一般制备方法: 硬模板法、软模板法以及自模板法, 并从合成方法的基本概念、合成步骤以及优缺点进行了概述. 总结了近年用于光催化领域中典型单一中空结构材料的合成方法和机理, 包括中空结构的CdS, Zn_xCd_1‒_xS, g-C₃N₄, TiO₂, CeO₂等体系. 但单一催化材料的光生电子-空穴对的复合效率较高, 导致其催化性能较低, 因此, 合理设计和构建多级结构对于提升光催化性能具有重要的意义. 其次, 对多级结构的中空材料进行了分类, 概述了构建策略、光催化制氢以及光催化还原二氧化碳的机制. 具有多级结构的中空光催化剂可分为两大类, 包括中空助催化剂为基体的材料和中空主光催化剂为基体的材料, 其它复杂中空光催体系也基于上述体系的延伸. 最后, 对中空结构的特征和影响规律的应用实例进行了介绍. 同时, 对文献报道的探索中空纳米材料光催化机理的有效方法, 如表面光电压测试、电子自旋顺磁共振技术、理论计算结合实验等技术手段进行了总结.
尽管中空材料在能量转换领域取得了一系列进展, 但该领域仍然存在诸多挑战, 与实际应用的要求仍然差距较大. 中空光催化材料的设计、制备和性能调控需要综合考虑经济、高性能、稳定性和环境友好等因素, 为大规模应用提供基础. 另一方面, 探索光催化机理非常重要, 深入进行机理研究不仅有利于设计高效光催化剂, 推动表征技术和微观结构分析的进步, 还有助于光催化领域的持续发展. 综上, 本文为新型中空材料的制备和光催化制氢和CO₂还原机理的深入探索提供一定的参考和依据.

关键词: 中空结构, 光催化, 制氢, CO₂还原, 设计原理

Abstract:

Photocatalysis is considered a prospective way to alleviate the energy crisis and environmental pollution. It is therefore extremely important to design highly efficient photocatalysts for catalytic systems. In recent years, hollow-structured materials have attracted considerable interest for application in energy conversion fields owing to their large specific surface areas, improved light absorption, and shortened charge carrier transfer path. Because they contain inner and outer surfaces, hollow-structured materials can provide a superior platform for the deposition of other components. A number of hollow-structured hierarchical systems have been designed and fabricated in recent decades. It is important to rationally design and construct complex hierarchical structures. In this review, general preparation approaches for hollow-structured materials are presented, followed by a summary of the recent synthesis methods and mechanisms of typical hollow-structured materials for applications in the photocatalytic field. Complex hollow-structured hierarchical photocatalysts are classified into two types, hollow cocatalyst-based and hollow host photocatalyst-based, and the design principle and analysis of the photocatalytic reaction mechanism for photocatalytic H₂ evolution and CO₂ reduction are also introduced. The effects of hollow-structured materials have also been investigated. This review provides a reference for the rational construction of advanced, highly efficient photocatalytic materials.

Key words: Hollow structure, Photocatalysis, H₂ evolution, CO₂ reduction, Design principle

李旭力, 李宁, 高旸钦, 戈磊. 中空纳米材料的构建原理及其在光催化制氢和二氧化碳还原反应中的应用[J]. 催化学报, 2022, 43(3): 679-707.

Xuli Li, Ning Li, Yangqin Gao, Lei Ge. Design and applications of hollow-structured nanomaterials for photocatalytic H₂ evolution and CO₂ reduction[J]. Chinese Journal of Catalysis, 2022, 43(3): 679-707.

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图/表 40

Fig. 1. Illustration of the advantages of hollow-structured materials.

Fig. 2. (a) Illustration of procedures for preparing inorganic and hybrid hollow spheres. (b) The scheme shown for PS latex particles. Reprinted with permission from Ref. [98]. Copyright 1998, American Association for the Advancement of Science.

Fig. 3. SEM (a) and TEM (b) images of solid PB mesocrystals (average particle size: 110 nm) as the starting material. SEM (c) and TEM (d) images of the hollow PB mesocrystals (average particle size: 110 nm) synthesized by chemical etching. Inset images on the SEM and TEM images are (a,c) enlarged SEM images of one particle and (b,d) the corresponding selected-area electron diffraction (SAED) patterns of one particle. Reprinted with permission from Ref. [110]. Copyright 2012, Wiley-VCH GmbH.

Fig. 4. Schematic illustration of the formation process of NiCo2S4 ball-in-ball hollow spheres. Stage I, surface NiCo2S4 formed by anion exchange method. Stage II, further diffusion of S2- and formation of NiCo2S4 on the inner NiCo-glycerate core. Stage III, completion of the anion exchange reaction. M2+ refers to metal cations, including Ni2+ and Co2+ ions. Reprinted with permission from Ref. [113]. Copyright 2015, Springer Nature.

Fig. 5. TEM images of core-shell ZIF-8@ZIF-67 NPs annealed at 500 °C (a,e), 550 °C (b,f), 600 °C (c,g), and 800 °C (d,h). (i) Schematic of the formation process of NC@Co-NGC DSNCs. Reprinted with permission from Ref. [115]. Copyright 2017, Wiley-VCH GmbH.

Table 1 The applications of CdS-based hollow structures in photocatalytic reactions.

Hollow photocatalyst	Morphology		Photocatalytic reaction	Performance (mmol h^-1 g^-1)	AQY	Year /Ref.
Hollow CdS			H₂ evolution	3.14	—	2019 [124]
CdS frame- in-cage particles			H₂ evolution	11.3	3.2%	2020 [136]
Double- shelled CdS			H₂ evolution	250.1	—	2020 [131]
Hollow CdS/Ni-Mo-S			H₂ evolution	838.17	—	2019 [134]
Hollow CdS/Co₉S₈			H₂ evolution	1061.3	—	2017 [199]
Hollow photocatalyst	Morphology	Photocatalytic reaction		Performance (mmol h^-1 g^-1)	AQY		Year /Ref.
Hollow CdS@g-C₃N₄		H₂ evolution		4.39	3.22% 420 nm		2018 [125]
CdS@ZnIn₂S₄ hollow cubes		H₂ evolution		540.3	1.53% 400 nm		2021 [221]
Pd@CdS/PdS		H₂ evolution		144.8	—		2018 [225]
MnO_x@CdS/ CoP		H₂ evolution		238.4 µmol h^-1 (10 mg)	—		2017 [226]
Au@HCS@ PdS		H₂ evolution		16.35	41% 420 nm		2020 [132]
Pt/TiO₂/CdS/ Co₃O₄		H₂ evolution		2000	—		2017 [228]
NG/CdS		CO₂ reduction		CO (2.59) CH₄ (0.33)	0.9% 420 nm		2019 [232]

Fig. 7. TEM images of the obtained products after reactions for 0.5, 2, and 4 h, and the corresponding schematic illustration of the formation process of CdS-H. Reprinted with permission from Ref. [135]. Copyright 2019, Royal Society of Chemistry.

Fig. 8. (a) Schematic illustration of the two-step sulfidation approach for the fabrication of CdS frame-in-cage particles. (b) TEM images of Cd-PBA cubes. (c,d) Cd-PBA cube-in-CdS cage particles. (e) CdS frame-in-cage particles. Reprinted with permission from Ref. [136]. Copyright 2020, Wiley-VCH GmbH.

Fig. 9. TEM (a) and HAADF-STEM and EDX mapping images (b) of Zn0.6Cd0.4S NPs. (c) Schematic illustration of the synthesis process of hollow ZnCdS cages. Reprinted with permission from Ref. [137]. Copyright 2017, Royal Society of Chemistry.

Fig. 10. (a) TEM images of AA-[Zn(OH)4]2- composite nanospheres. (b) TEM images of ZnS composite nanospheres. (c) TEM images of DS-Zn0.46Cd0.54S hollow nanospheres. (d) Schematic illustration of the synthetic strategy of ZnxCd1-xS double-shell hollow nanospheres. Reprinted with permission from Ref. [148]. Copyright 2018, Elsevier B.V.

Table 2 The applications of ZnxCd1-xS or ZnIn2S4-based hollow structures in photocatalytic reactions.

Hollow structure	Photocatalytic reaction	Performance (mmol h^-1 g^-1)	AQY (%)	Year /Ref.
Zn_xCd_1-_xS double-shell hollow nanospheres	H₂ evolution	4110	—	2018 [148]
Hollow ZnCdS	H₂ evolution	5.68	—	2017 [137]
Co₉S₈/ZCS	H₂ evolution	10.9	8.96 420 nm	2020 [201]
Co₉S₈/ZCS	H₂ evolution	9.039	4.49 420 nm	2020 [202]
Co₉S₈@ZnIn₂S₄	H₂ evolution	6.250	—	2018 [200]
Co/NGC@ ZnIn₂S₄	H₂ evolution	11.270	5.07 420 nm	2019 [210]
MoSe₂/CdSe	H₂ evolution O₂ evolution	7.120 0.348	27.2 670 nm	2019 [207]

Table 3 The applications of g-C3N4-based hollow structures in photocatalytic reactions.

Hollow structure	Photocatalytic reaction	Performance	AQY (%)	Year /Ref.
Co₃O₄/ HCNS/Pt	H₂ evolution O₂ evolution	0.3 µmol h^-1 0.1 µmol h^-1(20 mg)	—	2016 [155]
PtNi/g-C₃N₄	H₂ evolution	98.6 µmol h^-1(50 mg)	5.89 420 nm	2018 [158]
CoS_x/g-C₃N₄	H₂ evolution	629 µmol h^-1 g^-1	—	2018 [203]
CoNiS_x-CN	H₂ evolution	2366 μmol h^-1 g^-1	4.3 420 nm	2019 [204]
g-C₃N₄@HG	H₂ evolution	1.43 mmol h^-1 g^-1	3.56 420 nm	2020 [188]

Fig. 11. (a,b) SEM images of the tubular g-C3N4 at different magnifications. (c) TEM image of tubular g-C3N4. (d) TEM image of single tube of tubular g-C3N4 (the inset is SAED pattern of tubular g-C3N4). From Ref. [161]. (e) Schematic illustration of the formation of the carbon nitride nanotubes. Reprinted with permission from Ref. [160]. Copyright 2013 and 2012, Royal Society of Chemistry.

Table 4 The applications of TiO2-based hollow structures in photocatalytic reactions.

Hollow structure	Photocatalytic reaction	Performance (mmol h^-1 g^-1)	AQY (%)	Year /Ref.
Co_1.62Mo₆S₈/THS	H₂ evolution	44.43	4.88 365 nm	2020 [171]
TiO₂/NiO	H₂ evolution dye degradation	393 µmol h^-1 g^-1 88% within 100 min	—	2015 [97]
NiO/TiO₂/C	H₂ evolution dye degradation	356 µmol h^-1 g^-1 RhB (94%) within 75 min MB (98%) within 100 min	—	2016 [220]
RuO₂@TiO₂@Pt	H₂ production Pollutant degradation	809 µmol h^-1 g^-1 RhB (98%); MO (80%) phenol (40%)	—	2016 [222]
Ag-I-RuO₂-O-THS	H₂ evolution	300.2 µmol (5 h, 80 mg)	—	2017 [223]
Pt@TiO₂@ MnO_x	O₂ evolution	31.22 mmol (14 h, 30 mg)	63.14 254 nm	2016 [224]
Au_x@THS@CoO	CO₂ reduction	CH₄ (13.3)	—	2019 [233]

Fig. 12. Representative TEM images of particles obtained after processing times of 1 h (a), 2 h (b), 3 h (c), 4 h (d), 5 h (e), and 7 h (f). (g) Schematic of the particle formation and development of the hollow structure in the solvothermal process. The chemical conversion caused nonuniform development of tiny grains and empty spaces within the spheres, which enhanced the outward migration and relocation of the core grains toward the outer layer, resulting in the generation and development of a hollow structure. Reprinted with permission from Ref. [174]. Copyright 2016, Elsevier B.V.

Fig. 13. TEM images showing the morphological evolution of sSiO2@TiO2 samples after hydrothermal treatment at 140 °C for 0 h (a), 1 h (b), 2 h (c), 5 h (d), 10 h (e), and 24 h (f,g). (h) SEM image of DHS-Ti. (i) SEM image showing a broken double-shelled structure. (j) Schematic illustration of the formation process of double-shelled TiO2 hollow spheres. Reprinted with permission from Ref. [175]. Copyright 2017, Wiley-VCH GmbH.

Table 5 The applications of CeO2-based or other hollow structures in photocatalytic reactions.

Hollow structures	Photocatalytic reaction	Performance (µmol h^-1 g^-1)	AQY (%)	Year /Ref.
CeO₂/ZnIn₂S₄	Benzaldehyde evolution H₂ evolution	664.1 1496.6	—	2020 [218]
CeO_2-_xS_x@CdS	H₂ evolution	1147.2	—	2019 [219]
g-C₃N₄@CeO₂	CO₂ reduction	CH₄ (3.5 µmol g^-1, 4 h) CH₃OH (5.2 µmol g^-1, 4 h) CO (16.8 µmol g^-1, 4 h)	17.1 525 nm	2019 [231]
ZnO_1-_x/C	CO₂ reduction	CO (µmol h^-1 g^-1, 4 h)	0.13	2018 [230]

Fig. 14. HRTEM and SAED images of CeO2 hollow structures: (a1,b1) polyhedron. (a2,b2) cube. (a3,b3) sphere. (c) Schematic illustration of the formation of CeO2 hollow structures by template-engaged coordinating etching of Cu2O nanocubes. Reprinted with permission from Ref. [183]. Copyright 2015, Elsevier B.V.

Fig. 15. (a) Schematic illustration of the synthetic process of hierarchical Co9S8@ZnIn2S4 heterostructured cage: (I) sulfidation reaction and thermal treatment in argon atmosphere and (II) growth of ZnIn2S4 nanosheets (NSs). (b) TEM images of Co9S8@ZnIn2S4 cages, (c) Photocatalytic H2 evolution performance of different samples. (d) EIS spectra of Co9S8@ZnIn2S4. Reprinted with permission from Ref. [200]. Copyright 2018, American Chemical Society.

Fig. 16. TEM images of CoSx (a), Co9S8 (b), and 10Co9S8/ZCS (c). (d) Photocatalytic H2 activity of different samples under visible-light irradiation. ESR spectra of h+ (e) and e- (f) signal of Zn0.5Cd0.5S and 10Co9S8/ZCS photocatalysts at different irradiation times at room temperature. (g) Work functions of Zn0.5Cd0.5S and Co9S8 samples. (h) Proposed mechanism of photocatalytic hydrogen process over Co9S8/ZCS composite. Reprinted with permission from Ref. [201]. Copyright 2020, Elsevier B.V.

Fig. 17. SEM (a) and TEM (b,c) images of the prepared 10%-Co9S8/ZnIn2S4 composite. (d) Schematic illustration of the fabrication process of hierarchical Co9S8/ZnIn2S4 tubular photocatalyst. (e) Amounts of H2 generated from the prepared samples in 5 h under visible-light irradiation. (f) Photocatalytic reduction of aqueous Cr(VI) by as-prepared samples under visible-light irradiation. (g) Schematic illustration of the transfer process of the photogenerated electrons and holes in the Co9S8/ZnIn2S4 heterostructure, and the photocatalytic mechanism for Cr(VI) reduction and H2 evolution under visible-light irradiation. Reprinted with permission from Ref. [202]. Copyright 2020,Wiley-VCH GmbH.

Fig. 18. (a) The schematic illustration for the fabrication of CoSx/g-C3N4 composites. TEM images of hollow CoSx polyhedrons (b) and 2%CoSx/g-C3N4 composite (c). (d) Photocatalytic H2 generation rate of g-C3N4 and CoSx/g-C3N4 composites with different CoSx contents (1% to 10%) under visible-light (λ ≥ 400 nm) irradiation. Electrostatic potentials of the monolayer g-C3N4 surface (e) and the CoS (001) surface (f). (g) The 3D charge density difference for CoS/g-C3N4 composite model. The isosurface value is 0.0004 e/Å3. The yellow and cyan regions represent charge accumulation and depletion, respectively. (h) The possible mechanism for the photocatalytic H2 evolution over the CoSx/g-C3N4 composite photocatalyst. (i) The schemes of light path and photothermal effect in the hollow CoSx polyhedron. Reprinted with permission from Ref. [203]. Copyright 2018, American Chemical Society.

Fig. 19. Electrostatic potentials for monolayer g-C3N4 (a) and CoNiSx (b). (c) Charge density difference of CoNiSx-CN model. The yellow regions represent charge accumulation, whereas the cyan regions represent charge depletion. (d) Calculated free-energy diagram of photocatalytic HER for the photocatalysts. Reprinted with permission from Ref. [204]. Copyright 2019, American Chemical Society.

Fig. 20. (a) SEM (A, B, D, E, G, H, J and K) and TEM (C, F, I and L) images of MoSe2 nanospheres with different reaction times (M1: 1 h; M2: 6 h; M3: 12 h; M4: 36 h) at 180 °C. (b-d) The photocatalytic mechanism of MoSe2/CdSe heterostructure with different light irradiation wavelengths. Reprinted with permission from Ref. [207]. Copyright 2019, Elsevier B.V.

Fig. 21. (a) TEM images of Co/NGC@ZIS cages. (b) Schematic illustration for the synthetic process of hierarchical Co/NGC@ZIS cages. I: growth of ZIF-67 on ZIF-8 particles. II: carbonization in N2 and acid etching. III: growth of ZnIn2S4 NSs. (c) Photocatalytic H2 evolution activities of Co/NGC, Co/NGC@ZIS, ZnIn2S4, and p-Co/NGC@ZIS. (d) H2 production rates of Co/NGC@ZIS with varied compositions, the solid counterparts of Co/NGC@ZIS-S and NGC@ZIS-S, and Co3O4/NGC@ZIS. (e) Illustration of the photocatalytic H2 evolution mechanism on Co/NGC@ZIS under visible-light irradiation. Reprinted with permission from Ref. [210]. Copyright 2019, Wiley-VCH GmbH.

Fig. 22. TEM (a), magnified TEM (b,c) and HRTEM (d) images of MHMs. (e) EDS mapping of multi-shelled hollow Cu-CeO2 microspheres. Reprinted with permission from Ref. [213]. Copyright 2019, Elsevier B.V. (f,g) TEM images of Pd@void@Pt@CeO2 core@shell nanospheres. (h,i) TEM images of (Pt-enriched cage)@CeO2 core@shell nanospheres. Reprinted with permission from Ref. [215]. Copyright 2017, Wiley-VCH GmbH.

Fig. 23. (a-c) TEM images of CeO2/ZnIn2S4. (d) Rates of photocatalytic dehydrogenation of PhCH2OH for H2 evolution and PhCHO production with different catalysts with a reaction time of 3 h. EPR spectra of DMPO-%O2- (e) and DMPO-%OH (f) over CeO2, ZnIn2S4, and CeO2/ZnIn2S4 under solar exposure. (g) Charge carrier flow mechanisms over Type II and direct Z-scheme heterojunctions for the CeO2/ZnIn2S4 composite. Reprinted with permission from Ref. [218]. Copyright 2020, Elsevier B.V.

Fig. 24. (a) Schematic illustration of the synthetic procedures for CdS@ZnIn2S4 hollow cubes (direct Z-scheme heterojunction). FESEM (b) and TEM (c) images. Reprinted with permission from Ref. [221]. Copyright 2021, Elsevier B.V.

Fig. 25. (a) TEM image of Pd@CdS/1%PdS. (b) An illustration of the preparation of Pd@CdS/PdS catalyst. (c) Time courses of H2 evolution over Pd@CdS/1%PdS. (d) Proposed charge transfer mechanism of the Pd@CdS/PdS catalyst. Reprinted with permission from Ref. [225]. Copyright 2018, Wiley-VCH GmbH.

Fig. 26. (a) TEM image of Au@HCS@PdS. (b) Schematic illustration for the formation of Au@HCS@PdS photocatalyst. (c) The comparison of enhancement of hydrogen production with the optimal amount of cocatalysts. (d,e) Arrhenius plots obtained by fitting the rates of photocatalytic hydrogen and temperature. The apparent activation energies were calculated with the Arrhenius equation. (f) Schematic diagram of photocatalytic H2 evolution mechanism on Au@HCS@PdS composite under visible-light irradiation. Reprinted with permission from Ref. [132]. Copyright 2020, Elsevier B.V.

Fig. 27. SEM (a) and TEM (b) images of HCNS/Pt samples. (c) TEM and HRTEM images of Co3O4/HCNS/Pt samples. (d) Time courses of photocatalytic evolution of H2 and O2 using Co3O4/HCNS/Pt (e) and (Co3O4+Pt)/HCNS (f) under UV irradiation (λ > 300 nm). Reprinted with permission from Ref. [155]. Copyright 2016, Wiley-VCH GmbH.

Fig. 28. (a) TEM image of Pt/TiO2/CdS/Co3O4 hollow spheres. (b) schematic of the synthesis process of Pt/TiO2/CdS/Co3O4 composite hollow spheres; Illustration of the (c) structure and (d) reaction procedure of double-shelled hollow sphere photocatalyst. Schematic of (e) band structures in TiO2/CdS double-shelled hollow spheres and (f) activity energy reduction on the surface of photocatalyst with Pt and Co3O4 Co-catalyst. Reprinted with permission from Ref. [228]. Copyright 2017, Elsevier B.V.

Fig. 29. (a,b) TEM images of CdG2. (c) Photocatalytic CO2 reduction performance of CdS, CdG1, CdG2, CdG3, and CdG5. (d) Schematic illustration of NG/CdS HS preparation process. Reprinted with permission from Ref. [232]. Copyright 2019, Wiley-VCH GmbH.

Fig. 30. (a,b) TEM image of Au2.0@THS@CoO. (c) Illustrations of formation process of Aux@THS@CoO. (d) Comparison of the average formation rates of CH4 for THS, THS@CoO, and Au2.0@THS@CoO samples. (e) EPR spectra of Au2.0@THS@CoO in the presence of CO2 and N2 before and after simulated solar light irradiation. (f) In situ FTIR spectra of CO2 and H2O interaction with Au2.0@THS@CoO and THS in the dark and subsequently irradiated for different times. (g) The possible mechanism for photoreduction CO2 over Aux@THS@CoO. Reprinted with permission from Ref. [233]. Copyright 2019, Elsevier B.V.

Fig. 31. (a) Schematic illustration of the formation process of NiCo2O4 hollow microspheres composed of nanosheets. TEM images of (b) NiCoG, (c) NiCo-OH and (d) NiCo2O4 hollow spheres. (e) EPR spectra of NiCo2O4 hollow spheres and NiCo2O4 nanoparticles. (f) CO2 adsorption isotherms of NiCo2O4 hollow spheres and NiCo2O4 nanoparticles at 273.15?K. (g) CO and H2 generation from the photocatalyst system under different reaction conditions and the percentages of the CO selectivity of different catalysts. (h) Time courses and stability tests of CO and H2 production over NiCo2O4 hollow spheres. Reprinted with permission from Ref. [235]. Copyright 2019, Elsevier B.V.

Fig. 32. (a) TEM image of 120BB. (b,c) In situ FTIR spectra of CO2 and H2O reaction on 120BB. (d) In situ ESR spectra of 120BB in different situations. (e,f) Electron densities of BiOBr and BiOBr (OVs) by DFT calculation. (g) Proposed mechanism of CO2 photoreduction for BiOBr microspheres. Reprinted with permission from Ref. [236]. Copyright 2021, Elsevier B.V.

Fig. 33. High‐resolution XPS spectra of N 1s (a) and Pt 4f (b). (c) CO2 TPD curves for the HHBs, N‐HHBs, and Pt/N‐HHBs. (d) Photocatalytic mechanism scheme of Pt1/N0.25‐HHBs under simulated sunlight irradiation. Reprinted with permission from Ref. [238]. Copyright 2020, Elsevier B.V.

Fig. 34. An overview of hollow materials for energy conversion.

Fig. 35. Development of hollow materials architecture.

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中空纳米材料的构建原理及其在光催化制氢和二氧化碳还原反应中的应用

Design and applications of hollow-structured nanomaterials for photocatalytic H₂ evolution and CO₂ reduction

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中空纳米材料的构建原理及其在光催化制氢和二氧化碳还原反应中的应用

Design and applications of hollow-structured nanomaterials for photocatalytic H2 evolution and CO2 reduction

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Design and applications of hollow-structured nanomaterials for photocatalytic H₂ evolution and CO₂ reduction