具有高效电荷转移的W18O49/CdSe-二乙烯三胺光催化CO2转化: LSPR效应和S型异质结协同效应

doi:10.1016/S1872-2067(21)64024-X

催化学报 ›› 2022, Vol. 43 ›› Issue (10): 2539-2547.DOI: 10.1016/S1872-2067(21)64024-X

具有高效电荷转移的W₁₈O₄₉/CdSe-二乙烯三胺光催化CO₂转化: LSPR效应和S型异质结协同效应

黄悦^a, 代凯^a^,^*(), 张金锋^a^,^#(), Graham Dawson^b

^a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, 安徽淮北 235000
^b西交利物浦大学化学系, 江苏苏州 215123

收稿日期:2021-12-14 接受日期:2022-01-15 出版日期:2022-10-18 发布日期:2022-09-30
通讯作者: 代凯,张金锋
基金资助:
国家自然科学基金(51572103);国家自然科学基金(51973078);安徽省杰出青年基金(1808085J14);安徽省教育厅重大项目(KJ2020ZD005);安徽省教育厅重点项目(KJ2019A0595)

Photocatalytic CO₂ conversion of W₁₈O₄₉/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction

Yue Huang^a, Kai Dai^a^,^*(), Jinfeng Zhang^a^,^#(), Graham Dawson^b

^aKey Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, College of Physics and Electronic Information, Huaibei Normal University, Huaibei 235000, Anhui, China
^bDepartment of Chemistry, Xi’an Jiaotong-Liverpool University, Suzhou 215123, Jiangsu, China

Received:2021-12-14 Accepted:2022-01-15 Online:2022-10-18 Published:2022-09-30
Contact: Kai Dai, Jinfeng Zhang
Supported by:
National Natural Science Foundation of China(51572103);National Natural Science Foundation of China(51973078);Distinguished Young Scholar of Anhui Province(1808085J14);Major projects of Education Department of Anhui Province(KJ2020ZD005);Key Foundation of Educational Commission of Anhui Province(KJ2019A0595)

摘要/Abstract

摘要：

近年来, 随着化石燃料消耗的急剧增加,排放到大气中的CO₂日益增多, 其导致的温室效应和环境污染问题日益突出, 因此如何实现CO₂高效转化利用成为当务之急. 光催化CO₂还原(PCR)技术是解决温室效应的策略之一. 目前, 大部分光催化剂的研究集中在提高可见光范围内的光催化活性, 如果开发出能够吸收和利用近红外(NIR)光的半导体光催化剂, 将可大幅提高太阳光的利用率, 从而提高PCR活性. 非化学计量的W₁₈O₄₉ (WO)由于氧空位引起的局部表面等离子体共振(LSPR)效应而具有较好的NIR吸收性. 此外, 氧空位引起的LSPR效应可以吸收低能光子, 并产生高能"热电子"以促进载流子转移, 可以改善光生电荷分离. 通过胺化的CdSe-二乙烯三胺(CdSe-D)和WO耦合构建S型异质结光催化剂, 可以提高光生载流子的分离效率. 因此, 该类结构在利用太阳光将CO₂转化为有机燃料的领域具有巨大的潜力.

本文通过溶剂热法在CdSe-D上原位生长WO. 采用X射线衍射(XRD)技术研究了不同比例的CdSe-D, WO和复合样品的物相, 没有观察到杂质峰, 表明没有其它杂质混入. 扫描电子显微镜和透射电子显微镜表结果表明, CdSe-D上的WO是原位生长的, 而不是简单的机械混合. 采用XPS光谱分析了WO, CdSe-D和35%WO/CdSe-D中的Cd, Se, O和W元素, 结果表明, 电子是从CdSe-D移动到WO. 根据UV-vis DRS结果, WO在450‒1800 nm有吸收峰, 这可归因于WO是一种非化学计量的氧化钨, 表面上有大量的氧空位, 从而触发了由电子集体振荡引起的LSPR效应. CdSe-D和WO带隙分别为1.97和2.68 eV. 由Mott-Schottky曲线对CdSe-D和WO的导带位置进行估计, 可以得出CdSe-D和WO的导带位置. 利用PL光谱、瞬态光电流响应和阻抗研究了光催化剂的界面电荷载流子转移和分离效率, 表明构建S型异质结加快电子的传输进一步提高了电荷分离和转移效率. 光催化CO₂还原测试可以发现, 35%WO/CdSe-D的产率为29.72 μmol h^-1 g^-1, 表现出最优异的CO₂还原性能, 且经过三次循环实验依然保持良好的光催化性能. 综上, 本文成功构建了胺化S型WO/CdSe-D异质结光催化剂, 光吸收范围增大, 光吸收能力增强, 氧化还原能力提高, 对具有富氧空位的非化学计量氧化物的LSPR效应提供了一种新的见解.

关键词: S型异质结, 光催化CO₂还原, W₁₈O₄₉, 表面等离子体共振, 二乙烯三胺

Abstract:

Non-stoichiometric W₁₈O₄₉ (WO) prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies. This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels. In addition, through the amination of CdSe, the one-dimensional/two-dimensional step-scheme (S-scheme) WO/CdSe-diethylenetriamine (WO/CdSe-D) photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method. The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency. The optimized photocatalyst of 35%WO/CdSe-D has the best CO₂ reduction performance compared to WO and CdSe-D, and the yield is 25.37 µmol h^-1 g^-1. X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction. This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO₂ reduction.

Key words: S-Scheme, Photocatalytic CO₂ reduction, W₁₈O₄₉, Localized surface plasmon resonance, Diethylenetriamine

黄悦, 代凯, 张金锋, Graham Dawson. 具有高效电荷转移的W₁₈O₄₉/CdSe-二乙烯三胺光催化CO₂转化: LSPR效应和S型异质结协同效应[J]. 催化学报, 2022, 43(10): 2539-2547.

Yue Huang, Kai Dai, Jinfeng Zhang, Graham Dawson. Photocatalytic CO₂ conversion of W₁₈O₄₉/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction[J]. Chinese Journal of Catalysis, 2022, 43(10): 2539-2547.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)64024-X

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图/表 11

Fig. 1. Schematic diagram of WO/CdSe-D compounding process.

Fig. 2. (a) XRD patterns of WO, and WO/CdSe-D. (b) XRD comparison patterns of CdSe-D and CdSe.

Fig. 3. TEM images of WO (a), CdSe-D (b) and 35%WO/CdSe-D (c). (d) HRTEM images of 35%WO/CdSe-D. SEM images of WO (e) and CdSe-D (f); TEM images of 35%WO/CdSe-D (g) and element mapping of Cd (h), O (i), Se (j) and W (k).

Fig. 4. (a) XPS full spectra of WO, CdSe-D and 35%WO/CdSe-D. High-resolution XPS of Cd 3d (b), Se 3d (c), W 4f (d) and O 1s (e).

Fig. 5. N2 adsorption-desorption isotherm curves (a) and SBET (b) of WO, CdSe-D and 35%WO/CdSe-D.

Fig. 6. (a) UV-Vis DRS of WO, CdSe-D and WO/CdSe-D. (b) plots of the (αhν)2 vs photon energy (hν) for WO and plots of the (αhν)1/2 vs. photon energy (hν) for CdSe-D; Mott-Schottky plots of (c) CdSe-D and (d) WO measured at the frequency of 2 and 3 kHz.

Fig. 7. PL spectra of WO, 35%WO/CdSe-D and CdSe-D.

Fig. 8. Transient photocurrent responses (a) and EIS (b) of CdSe-D, WO and 35%WO/CdSe-D.

Fig. 9. (a) PCR rate of CdSe-D, WO, WO/CdSe-D,WO+CdSe-D and 35% WO/CdSe; (b) Cyclic experiment results of CdSe-D, WO and WO/CdSe-D.

Fig. 10. Optimized structures of WO (100) (a) and CdSe (100) (b). Calculated Fermi energy levels and work functions of WO (100) (c) and CdSe (100) (d).

Fig. 11. Schematic diagram of the photocatalytic mechanism of the composite.

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具有高效电荷转移的W₁₈O₄₉/CdSe-二乙烯三胺光催化CO₂转化: LSPR效应和S型异质结协同效应

Photocatalytic CO₂ conversion of W₁₈O₄₉/CdSe-Diethylenetriamine with high charge transfer efficiency: Synergistic effect of LSPR effect and S-scheme heterojunction

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