LSPR效应增强碳包覆In2O3/W18O49 S型异质结用于高效CO2光还原

doi:10.1016/S1872-2067(23)64420-1

催化学报 ›› 2023, Vol. 48: 267-278.DOI: 10.1016/S1872-2067(23)64420-1

LSPR效应增强碳包覆In₂O₃/W₁₈O₄₉ S型异质结用于高效CO₂光还原

何厚伟¹, 王中辽¹, 代凯^*(), 李素文^*(), 张金锋^*()

淮北师范大学物理与电子信息学院, 绿色和精准合成化学及应用教育部重点实验室, 污染物敏感材料与环境修复安徽省重点实验室, 安徽淮北235000

收稿日期:2023-01-18 接受日期:2023-02-28 出版日期:2023-05-18 发布日期:2023-04-20
通讯作者: * 电子信箱: daikai940@chnu.edu.cn (代凯), swli@chnu.edu.cn (李素文), jfzhang@chnu.edu.cn (张金锋).
作者简介:第一联系人：
¹共同第一作者
基金资助:
国家自然科学基金(22278169);国家自然科学基金(51973078);安徽省高校优秀科研创新团队(2022AH010028);安徽省教育厅重大项目(2022AH040068)

LSPR-enhanced carbon-coated In₂O₃/W₁₈O₄₉ S-scheme heterojunction for efficient CO₂ photoreduction

Houwei He¹, Zhongliao Wang¹, Kai Dai^*(), Suwen Li^*(), Jinfeng Zhang^*()

Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Anhui Province Key Laboratory of Pollutant SensitiveMaterials and Environmental Remediation, College of physics and Electron Information, Huaibei Normal University, Huaibei 235000, Anhui, China

Received:2023-01-18 Accepted:2023-02-28 Online:2023-05-18 Published:2023-04-20
Contact: * E-mail: daikai940@chnu.edu.cn (K. Dai), swli@chnu.edu.cn (S. Li), jfzhang@chnu.edu.cn (J. Zhang).
About author:First author contact:
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22278169);National Natural Science Foundation of China(51973078);Excellent scientific research and innovation team of Education Department of Anhui Province(2022AH010028);Major projects of Education Department of Anhui Province(2022AH040068)

摘要/Abstract

摘要：

太阳能驱动的光催化CO₂还原(PCR)技术可以将CO₂转化为增值燃料, 被认为是可以解决化石能源的日益减少和环境污染问题的可持续能源转换技术. CO₂的光催化还原涉及多种催化剂和反应途径, 构建异质结催化剂是提高光催化CO₂还原效率的重要策略. 然而, 异质结催化剂的光吸收范围一直是影响其性能的重要因素. 在增强近红外区光吸收的众多材料中, 具有局部表面等离子体共振(LSPR)效应的非贵金属等离子体材料是合适的选择. W₁₈O₄₉具有特殊的缺陷结构和LSPR效应, 可以产生高能"热电子"并促进载流子转移, 进一步优化了W₁₈O₄₉敏化光催化复合材料的设计, 在光催化中显示出非凡的潜力和研究价值.
本文在源自In-MOF的碳包覆In₂O₃(C-In₂O₃)纳米棒外表面组装一维高吸光度W₁₈O₄₉纳米线, 设计和制备C-In₂O₃/W₁₈O₄₉分级S型异质结. 采用X射线衍射、扫描电镜和透射电镜对样品进行了结构和形貌表征, 结果表明, 成功制备了C-In₂O₃/W₁₈O₄₉复合材料. 通过X射线光电子能谱和密度泛函理论计算分析了电子流向, 验证了S型异质结的机理. 使用原位漫反射红外傅里叶变换光谱、气相色谱和同位素标定进一步确定了PCR反应中间体活化过程和反应产物, 其中40%C-In₂O₃/W₁₈O₄₉复合材料的CO产率最高, 达到135.82 µmol·h^-1·g^-1, 分别是纯C-In₂O₃和W₁₈O₄₉的2.99和2.84倍. 采用时间分辨瞬态光致发光光谱测定样品的荧光寿命, 结果表明, C-In₂O₃/W₁₈O₄₉复合材料拥有更长的载流子衰变动力学的平均寿命(4.0707 ns), 表明复合材料可以更有效地利用可见光进行光催化反应.
C-In₂O₃/W₁₈O₄₉复合材料较好的催化性能主要归因于以下两个方面. (1) 碳涂层的高电子电导率促进了C-In₂O₃和W₁₈O₄₉之间的电荷转移, 载流子在非均相界面的均匀分布和高清的转移是光催化活性提高的重要原因; (2) S型异质结中的内部电子转移和注入C-In₂O₃的LSPR诱导的“热电子”实现了PCR的双路径电子转移, 从而使得PCR反应的活性得到了显著提高. 综上, 本文为开发高效可见光催化剂提供了新思路和实验依据.

关键词: 光催化CO₂还原, S型异质结, 局部表面等离子体共振, 碳包覆氧化铟, W₁₈O₄₉

Abstract:

The special defect structure and localized surface plasmon resonance (LSPR) effect offer W₁₈O₄₉ extraordinary potential and research value in photocatalysis. The LSPR effect optimizes the design of W₁₈O₄₉-sensitized photocatalytic composites and broadens the light-response range of W₁₈O₄₉. However, the high-energy “hot electrons” generated by W₁₈O₄₉ under the LSPR effect exhibit an extremely short lifetime and cannot be fully utilized. Therefore, the high electron conductivity of carbon can be used to increase the rate of hot-electron transfer, thereby extending the lifetime of hot electrons. In this study, a heterojunction photocatalyst was formed by growing a high-absorbance one-dimensional nanowire W₁₈O₄₉ on the surface of carbon-coated porous In₂O₃ nanorods (C-In₂O₃) derived from In-MOF. The C-In₂O₃/W₁₈O₄₉ composites exhibited optical responses in both the visible and near-infrared regions. The carbon coatings acted as transport channels to accelerate the transfer of carriers and hot electrons, and the activity of photocatalytic CO₂ reduction (PCR) was significantly enhanced. The 40%C-In₂O₃/W₁₈O₄₉ composites had the highest CO yield in the photocatalytic reactions, which was 2.99 and 2.84 times greater than that of pure C-In₂O₃ and W₁₈O₄₉, respectively. The internal electronic transfer in the S-scheme heterojunction and LSPR-induced hot electrons injected into C-In₂O₃ achieved dual-path electron transfer for PCR.

Key words: Photocatalytic CO₂ reduction, S-scheme heterojunction, Localized surface plasmon resonance, Carbon-coated In₂O₃, W₁₈O₄₉

何厚伟, 王中辽, 代凯, 李素文, 张金锋. LSPR效应增强碳包覆In₂O₃/W₁₈O₄₉ S型异质结用于高效CO₂光还原[J]. 催化学报, 2023, 48: 267-278.

Houwei He, Zhongliao Wang, Kai Dai, Suwen Li, Jinfeng Zhang. LSPR-enhanced carbon-coated In₂O₃/W₁₈O₄₉ S-scheme heterojunction for efficient CO₂ photoreduction[J]. Chinese Journal of Catalysis, 2023, 48: 267-278.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64420-1

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图/表 10

Fig. 1. Schematic diagram of the synthetic route of C-In2O3/W18O49 composites.

Fig. 2. SEM images of C-In2O3 (a), W18O49 (b), and 40%C-In2O3/W18O49 (c). (d) TEM image of C-In2O3. (e) HRTEM image of 40%C-In2O3/W18O49. (f-i) Element mapping images of C-In2O3/W18O49.

Fig. 3. (a) XRD patterns of In2O3, X%C-In2O3/W18O49, and W18O49. Full spectrum (b), C 1s (c), W 4f (d), In 3d (e), and O 1s (f) XPS spectra of samples.

Fig. 4. (a) UV-Vis diffuse reflectance spectra of different photocatalysts. (b) Plots of (αhν)2 versus energy (hν) for W18O49 and C-In2O3. (c,d) Mott-Schottky curve of W18O49 and C-In2O3. (e) Transient photocurrent response patterns of the photocatalysts. (f) EIS curves for C-In2O3, 40%C-In2O3/W18O49, and W18O49.

Fig. 5. (a) PL spectra of the prepared samples. (b) Time-resolved PL spectra.

Table 1 Dynamics analysis of the emission decay for different samples.

Sample	A₁ (%)	τ₁ (ns)	A₂ (%)	τ₂ (ns)	A₃ (%)	τ₃ (ns)	τ_A (ns)
W₁₈O₄₉	48.40	0.4861	34.87	2.4622	16.73	10.8105	2.9025
C-In₂O₃	59.21	0.5868	25.58	2.6342	15.21	11.9292	2.8358
C-In₂O₃/W₁₈O₄₉	49.56	0.8126	34.41	3.5399	19.02	13.4359	4.0707

Fig. 6. (a) Nitrogen adsorption/desorption isotherms. (b) BET specific surface area.

Fig. 7. (a) CO evolution rate of all the samples. (b) Performance cycle experiments. (c) Performance comparison of the catalysts with and without carbon coating. (d) CO evolution rate of the catalysts under different experimental conditions. (e,f) The mass spectroscopy analysis result of CO stemmed from the 13CO2 isotope experiment of 40%C-In2O3/W18O49 and in situ DRIFTS spectra.

Fig. 8. (a) Optimized structural models of W18O49 (100) and (b) In2O3 (100). (c,d) Calculated Fermi levels and work functions for W18O49 (100) and In2O3 (111).

Fig. 9. Photocatalytic mechanism of the C-In2O3/W18O49 composite under simulated sunlight illumination.

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LSPR效应增强碳包覆In₂O₃/W₁₈O₄₉ S型异质结用于高效CO₂光还原

LSPR-enhanced carbon-coated In₂O₃/W₁₈O₄₉ S-scheme heterojunction for efficient CO₂ photoreduction

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