W18O49/铝掺杂SrTiO3 S型异质结在LSPR效应辅助下实现全光谱太阳光驱动的光催化产氢

doi:10.1016/j.actphy.2025.100145

物理化学学报 >> 2025, Vol. 41 >> Issue (11): 100145.doi: 10.1016/j.actphy.2025.100145

W₁₈O₄₉/铝掺杂SrTiO₃ S型异质结在LSPR效应辅助下实现全光谱太阳光驱动的光催化产氢

蒋金辉¹^,†, 孙佳琦¹^,†, 陈咏一¹^,², 张磊¹^,², 董鹏玉¹^,*()

¹ 盐城工学院, 江苏省新型环保重点实验室, 江苏盐城 224051
² 盐城工学院材料科学与工程学院, 江苏省生态环境材料重点实验室, 江苏盐城 224051

收稿日期:2025-06-20 修回日期:2025-07-30 录用日期:2025-07-31 发布日期:2025-09-29
通讯作者: Email: dongpy11@gmail.com (董鹏玉)
作者简介:
^†These two authors contributed equally to this work (J.J. and J.S.).
基金资助:
国家自然科学基金(21403184); 中国江苏省高校自然科学研究基金(22KJA430008)

W₁₈O₄₉/Al-doped SrTiO₃ S-scheme heterojunction aided by the LSPR effect for full-spectrum solar light-driven photocatalytic hydrogen evolution

Jinhui Jiang¹, Jiaqi Sun¹, Yongyi Chen¹^,², Lei Zhang¹^,², Pengyu Dong¹^,*()

¹ Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China
² Key Laboratory for Ecological-Environment Materials of Jiangsu Province, School of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China

Received:2025-06-20 Revised:2025-07-30 Accepted:2025-07-31 Published:2025-09-29
Contact: Email: dongpy11@gmail.com (Pengyu Dong)
Supported by:
the National Natural Science Foundation of China(21403184); the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJA430008)

1. ACTPHY-2025.100145-SI-5p.pdf(1275KB)

摘要/Abstract

摘要：

开发具有全光谱响应的高效光催化剂用于制氢具有重要意义。为了实现全光谱太阳光驱动的光催化，W₁₈O₄₉由于局域表面等离子体共振(LSPR)效应，在捕获可见光和近红外(NIR)光方面表现良好。然而，W₁₈O₄₉的光催化产氢活性非常低，需要进行改性。在本研究中，采用简单的原位溶剂热合成方法制备了Al掺杂的SrTiO₃ (ASTO)/W₁₈O₄₉ S型异质结。得益于更强的载流子分离、更快的电子传输和强大的氧化还原能力，10% ASTO/W₁₈O₄₉ S型异质结表现出最高的全光谱太阳光驱动光催化产氢速率，分别是纯ASTO和W₁₈O₄₉的17.5倍和27.6倍。W₁₈O₄₉中丰富的氧空位产生的LSPR效应将光吸收范围扩展到NIR区域，显著提高了其对全光谱太阳光的利用效率。此外，由于W₁₈O₄₉的LSPR效应，它可以产生等离子体高能“热电子”，并使其转移到ASTO/W₁₈O₄₉异质结中ASTO的导带(CB)，从而促进光生载流子的分离和迁移，并大大增加ASTO的CB上参与光催化产氢反应的光生电子和“热电子”的数量，与单一组分的W₁₈O₄₉和ASTO相比，表现出优异的光催化产氢性能。

关键词: S型异质结, 光催化产氢, 局域表面等离子体共振效应, W₁₈O₄₉, 铝掺杂SrTiO₃

Abstract:

Developing highly efficient photocatalysts with a full-spectrum response for hydrogen production is of great significance. To achieve full-spectrum solar-light-driven photocatalysis, W₁₈O₄₉ works well for capturing visible and near-infrared (NIR) light due to the localized surface plasmon resonances (LSPR) effect. Nevertheless, W₁₈O₄₉ has very little photocatalytic hydrogen generation activity, which needs to be modified. In this work, a simple in situ solvothermal synthesis method was conducted to prepare Al-doped SrTiO₃ (ASTO)/W₁₈O₄₉ S-scheme heterojunction. Benefiting from more powerful carrier separation, faster electron transport, and strong redox capacity, the 10% ASTO/W₁₈O₄₉ S-scheme heterojunction exhibits the highest full-spectrum solar-light-driven photocatalytic hydrogen rate, which is 17.5 and 27.6 times that of pure ASTO and W₁₈O₄₉, respectively. The LSPR effect derived from W₁₈O₄₉ with abundant oxygen vacancies extends the range of light absorption to the NIR region, which significantly improves its utilization efficiency of full-spectrum sunlight. Moreover, due to the LSPR effect of W₁₈O₄₉, it could produce plasmonic high-energy "hot electrons" and allow them to transfer to the conduction band (CB) of ASTO in the ASTO/W₁₈O₄₉ heterojunction, which could promote the separation and migration of photoinduced carriers and greatly increase the number of electrons containing photogenerated electrons and "hot electrons" on the CB of ASTO that can participate in photocatalytic hydrogen production reaction, exhibiting excellent photocatalytic hydrogen evolution performance compared to single-component W₁₈O₄₉ and ASTO.

Key words: S-scheme heterojunction, Photocatalytic hydrogen evolution, LSPR effect, W₁₈O₄₉, Al-doped SrTiO₃

蒋金辉, 孙佳琦, 陈咏一, 张磊, 董鹏玉. W₁₈O₄₉/铝掺杂SrTiO₃ S型异质结在LSPR效应辅助下实现全光谱太阳光驱动的光催化产氢[J]. 物理化学学报, 2025, 41(11), 100145. doi: 10.1016/j.actphy.2025.100145

Jinhui Jiang, Jiaqi Sun, Yongyi Chen, Lei Zhang, Pengyu Dong. W₁₈O₄₉/Al-doped SrTiO₃ S-scheme heterojunction aided by the LSPR effect for full-spectrum solar light-driven photocatalytic hydrogen evolution[J]. Acta Phys. -Chim. Sin. 2025, 41(11), 100145. doi: 10.1016/j.actphy.2025.100145

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100145

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I11/100145

图/表 10

图1

图2

图3

图4

图5

图6

图7

图8

图9

参考文献 49

1	Wang Q.; Domen K. Chem. Rev. 2020, 120, 919. doi: 10.1021/acs.chemrev.9b00201
2	Wang Q.; Hisatomi T.; Jia Q.; Tokudome H.; Zhong M.; Wang C.; Pan Z.; Takata T.; Nakabayashi M.; Shibata N. et al. Nat. Mater. 2016, 15, 611. doi: 10.1038/nmat4589
3	Mu L.; Zhao Y.; Li A.; Wang S.; Wang Z.; Yang J.; Wang Y.; Liu T.; Chen R.; Zhu J.; et al Energy Environ. Sci. 2016, 9, 2463. doi: 10.1039/C6EE00526H
4	Zhang Y.; Wu X. F.; Wang Z. H.; Peng Y.; Liu Y. W.; Yang S.; Sun C. H.; Xu X. X.; Zhang X.; Kang J.; et al J. Am. Chem. Soc. 2024, 146, 6618. doi: 10.1021/jacs.3c12062
5	Wang C.; Jia Q.; Zhang X.; Chen X.; Wang Y.; Yu G.; Duan D. Small 2025, 21, 2407963. doi: 10.1002/smll.202407963
6	Qin Y. L.; Fang F.; Xie Z. Z.; Lin H. W.; Zhang K.; Yu X.; Chang K. ACS Catal. 2021, 11, 11429. doi: 10.1021/acscatal.1c02874
7	Goto Y.; Hisatomi T.; Wang Q.; Higashi T.; Ishikiriyama K.; Maeda T.; Sakata Y.; Okunaka S.; Tokudome H.; Katayama M. Joule 2018, 2, 509. doi: 10.1016/j.joule.2017.12.009
8	Takata T.; Jiang J. Z.; Sakata Y.; Nakabayashi M.; Shibata N.; Nandal V.; Seki K.; Hisatomi T.; Domen K. Nature 2020, 581, 411. doi: 10.1038/s41586-020-2278-9
9	Li R. H.; Takata T.; Zhang B. B.; Feng C.; Wu Q. B.; Cui C. H.; Zhang Z. M.; Domen K.; Li Y. B. Angew. Chem. Int. Ed. 2023, 62, e202313537. doi: 10.1002/anie.202313537
10	Wei Z.; Yan J.; Guo W.; Shangguan W. Chin. J. Catal. 2023, 48, 279. doi: 10.1016/S1872-2067(23)64414-6
11	Dong G.; Huang X.; Bi Y. Angew. Chem. Int. Ed. 2022, 61, e202204271. doi: 10.1002/anie.202204271
12	Zhang N.; Jalil A.; Wu D.; Chen S.; Liu Y.; Gao C.; Ye W.; Qi Z.; Ju H.; Wang C. et al. J. Am. Chem. Soc. 2018, 140, 9434. doi: 10.1021/jacs.8b02076
13	Bhavani P.; Kumar D. P.; Hussain M.; Jeon K.-J.; Park Y.-K. Catal. Rev. 2023, 65, 1521. doi: 10.1080/01614940.2022.2038472
14	Zhang Z.; Huang J.; Fang Y.; Zhang M.; Liu K.; Dong B. Adv. Mater. 2017, 29, 1606688. doi: 10.1002/adma.201606688
15	Yan J.; Wang T.; Wu G.; Dai W.; Guan N.; Li L.; Gong J. Adv. Mater. 2015, 27, 1580. doi: 10.1002/adma.201404792
16	Liu Y.; Zhang Z.; Fang Y.; Liu B.; Huang J.; Miao F.; Bao Y.; Dong B. Appl. Catal. B: Environ. 2019, 252, 164. doi: 10.1016/j.apcatb.2019.04.035
17	Meng K.; Zhang J.; Cheng B.; Ren X.; Xia Z.; Xu F.; Zhang L.; Yu J. Adv. Mater. 2024, 36, 2406460. doi: 10.1002/adma.202406460
18	Sayed M.; Yu J.; Liu G.; Jaroniec M. Chem. Rev. 2022, 122, 10484. doi: 10.1021/acs.chemrev.1c00473
19	He H.; Wang Z.; Dai K.; Li S.; Zhang J. Chin. J. Catal. 2023, 48, 267. doi: 10.1016/S1872-2067(23)64420-1
20	Liu Q.; He X.; Peng J.; Yu X.; Tang H.; Zhang J. Chin. J. Catal. 2021, 42, 1478. doi: 10.1016/S1872-2067(20)63753-6
21	Zhu B.; Sun J.; Zhao Y.; Zhang L.; Yu J. Adv. Mater. 2024, 36, 2310600. doi: 10.1002/adma.202310600
22	Zhang L.; Zhang J.; Yu J.; García H. Nat. Rev. Chem. 2025, 9, 328. doi: 10.1038/s41570-025-00698-3
23	Li S.; Wang Y.; Wang J.; Kirk C. H.; Wang H.; Sun J.; Liu Y.; Liu B.; Zhang T.; Jiang S.; et al Chem. Eng. J. 2023, 466, 143184. doi: 10.1016/j.cej.2023.143184
24	Chen J.; Bai P.; Yuan S.; He Y.; Niu Z.; Zhao Y.; Li Y. Chin. J. Catal. 2024, 67, 124. doi: 10.1016/S1872-2067(24)60149-X
25	Zhang J.; Yu W.; Zhang Y.; Zhu J. Int. J. Hydrogen Energy 2024, 85, 165. doi: 10.1016/j.ijhydene.2024.08.266
26	Huang Y.; Dai K.; Zhang J.; Dawson G. Chin. J. Catal. 2022, 43, 2539. doi: 10.1016/S1872-2067(21)64024-X
27	Liu Q.; He X.; Tao J.; Tang H.; Liu Z.-Q. ChemNanoMat 2021, 7, 44. doi: 10.1002/cnma.202000536
28	Liu H.-Y.; Niu C.-G.; Guo H.; Huang D.-W.; Liang C.; Yang Y.-Y.; Tang N.; Zhang X.-G. J. Colloid Interf. Sci. 2022, 610, 953. doi: 10.1016/j.jcis.2021.11.141
29	Xue W.; Sun H.; Hu X.; Bai X.; Fan J.; Liu E. Chin. J. Catal. 2022, 43, 234. doi: 10.1016/S1872-2067(20)63783-4
30	Yang Y.; Qiu M.; Qi Q.; Chen F.; Chen J.; Liu Y.; Yang L. ACS Appl. Nano Mater. 2020, 3, 10296. doi: 10.1021/acsanm.0c02210
31	Saadetnejad D.; Yıldırım R. Int. J. Hydrogen Energy 2018, 43, 1116. doi: 10.1016/j.ijhydene.2017.10.154
32	Gao K.; Li K.; Pan J.; Wang C.; Zhang L.; Wang W.; Xi X.; Dong P. Appl. Surf. Sci. 2024, 644, 158794. doi: 10.1016/j.apsusc.2023.158794
33	Xia Y.; He Z.; Su J.; Liu Y.; Tang B. Nanoscale Res. Lett. 2018, 13, 148. doi: 10.1186/s11671-018-2558-6
34	Duan M.; Hu C.; Li H.; Chen Y.; Chen R.; Gong W.; Lu Z.; Zhang N.; Long R.; Song L.; et al JACS Au 2022, 2, 1160. doi: 10.1021/jacsau.2c00146
35	Lu Y.; Jia X.; Ma Z.; Li Y.; Yue S.; Liu X.; Zhang J. Adv. Funct. Mater. 2022, 32, 2203638. doi: 10.1002/adfm.202203638
36	Xiao X.; Gao Y.; Zhang L.; Zhang J.; Zhang Q.; Li Q.; Bao H.; Zhou J.; Miao S.; Chen N.; et al Adv. Mater. 2020, 32, 2003082. doi: 10.1002/adma.202003082
37	Dong P.; Gao K.; Zhang L.; Huan H.; Xie M.-H.; Yang X.-L.; Zhang J. Appl. Catal. B: Environ. Energy 2024, 357, 124297. doi: 10.1016/j.apcatb.2024.124297
38	Liu J.; Liu Y.; Liu N.; Han Y.; Zhang X.; Huang H.; Lifshitz Y.; Lee S.-T.; Zhong J.; Kang Z. Science 2015, 347, 970. doi: 10.1126/science.aaa5760
39	Dong P.; Wang Y.; Zhang A.; Cheng T.; Xi X.; Zhang J. ACS Catal. 2021, 11, 13266. doi: 10.1021/acscatal.1c03441
40	Hou Y.; Du X.; Scheiner S.; McMeekin D. P.; Wang Z.; Li N.; Killian M. S.; Chen H.; Richter M.; Levchuk I.; et al Science. 2017, 358, 1192. doi: 10.1126/science.aao5561
41	Wang S. C.; Chen P.; Bai Y.; Yun J. H.; Liu G.; Wang L. Z. Adv. Mater. 2018, 30, 1800486. doi: 10.1002/adma.201800486
42	Qiu J.; Meng K.; Zhang Y.; Cheng B.; Zhang J.; Wang L.; Yu J. Adv. Mater. 2024, 36, 2400288. doi: 10.1002/adma.202400288
43	Guo H.; Jiang J.; Liang J.; Wen C.; Xi X.; Dong P. Chem. Eng. J. 2025, 504, 158649. doi: 10.1016/j.cej.2024.158649
44	Zhou Y.; Dong P.; Liu J.; Zhang B.; Zhang B.; Xi X.; Zhang J. Adv. Funct. Mater. 2025, 2500733. doi: 10.1002/adfm.202500733
45	Wang S.-D.; Huang L.-Y.; Xue L.-J.; Kang Q.; Wen L.-L.; Lv K.-L. Appl. Catal. B: Environ. Energy 2024, 358, 124366. doi: 10.1016/j.apcatb.2024.124366
46	Bai J.; Shen R.; Jiang Z.; Zhang P.; Li Y.; Li X. Chin. J. Catal. 2022, 43, 359. doi: 10.1016/S1872-2067(21)63883-4
47	Gu Y.; Li Y.; Feng H.; Han Y.; Li Z. Nano Res. 2024, 17, 4961. doi: 10.1007/s12274-024-6501-0
48	Gu M.; Zhang J.; Kurganskii I. V.; Poryvaev A. S.; Fedin M. V.; Cheng B.; Yu J.; Zhang L. Adv. Mater. 2025, 37, 2414803. doi: 10.1002/adma.202414803
49	Cai J.; Cheng C.; Liu B.; Zhang J.; Jiang C.; Cheng B. Acta Phys. Chim. Sin. 2025, 41, 100084. doi: 10.1016/j.actphy.2025.100084

[1]	樊凡, 修浩, 王宇婷, 崔永朋, 王雅君. NH₂-MIL-125/Na掺杂g-C₃N₄复合S型异质结的构建及其光催化产过氧化氢性能[J]. 物理化学学报, 2026, 42(2): 100143 - .
[2]	葛成艳, 胡佳伟, 刘星雨, 宋玉玺, 刘超, 邹志刚. 自集成黑色NiO团簇与ZnIn₂S₄微球实现S型电子转移机制下光热辅助制氢[J]. 物理化学学报, 2026, 42(1): 100154 - .
[3]	陈轼逸, 付家龙, 裘建平, 常国菊, 郝仕油. 废弃医用口罩衍生的碳量子点增强BiOBr/g-C₃N₄ S型异质结光催化降解聚对苯二甲酸乙二醇酯(PET)[J]. 物理化学学报, 2026, 42(1): 100135 - .
[4]	韦梦兰, 欧晓霞, 王艺濛, 张梦圆, 滕飞, 王凯旋. S型异质结g-C₃N₄/Bi₂WO₆高效降解左氧氟沙星：性能、机理及降解路径[J]. 物理化学学报, 2025, 41(9): 100105 - .
[5]	王文龙, 郝文韬, 何浪, 乔佳, 李宁, 陈朝秋, 覃勇. 碳量子点/TiO₂ S型异质结的能带和吸附工程促进光催化CO₂甲烷化[J]. 物理化学学报, 2025, 41(9): 100116 - .
[6]	蔡家杰, 程畅, 刘博文, 张建军, 姜传佳, 程蓓. CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学[J]. 物理化学学报, 2025, 41(8): 100084 - .
[7]	孟凡鹏, 赵飞, 林靖恺, 赵金生, 张华阳, 王少彬. 优化氮化碳纳米片/球形共轭聚合物S型异质结界面电场以促进析氢反应[J]. 物理化学学报, 2025, 41(8): 100095 - .
[8]	王伟康, 吴亚栋, 张建军, 孟凯, 李金河, 王乐乐, 刘芹芹. 三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H₂O₂合成：协同界面电荷转移调控与局域光热效应[J]. 物理化学学报, 2025, 41(8): 100093 - .
[9]	苗鑫宇, 杨浩, 何杰, 王晶, 靳治良. 调整Keggin型多金属氧酸盐电子结构构建S型异质结用于光催化析氢[J]. 物理化学学报, 2025, 41(6): 100051 - .
[10]	杨祎, 周欣, 谷苗莉, 程蓓, 吴珍, 张建军. S型ZnO/CdIn₂S₄光催化剂制备H₂O₂偶联苄胺氧化的超快电子转移飞秒吸收光谱研究[J]. 物理化学学报, 2025, 41(6): 100064 - .
[11]	李朋, 崔元映, 王中辽, DawsonGraham, 邵春风, 代凯. CeO₂/Bi₁₉Br₃S₂₇ S型异质结的高效界面电荷转移用于增强光催化CO₂还原[J]. 物理化学学报, 2025, 41(6): 100065 - .
[12]	吴金往, 谢琦靖, 张成亮, 史海峰. 自旋极化增强ZnFe_1.2Co_0.8O₄/BiVO₄ S型异质结光催化性能降解四环素[J]. 物理化学学报, 2025, 41(5): 100050 - .
[13]	马德运, 梁凤兰, 薛清泉, 刘艳萍, 庄春强, 李世杰. 界面工程与氧空位协同策略促进Cd_0.5Zn_0.5S/BiOBr S型异质结高效光催化去除抗生素[J]. 物理化学学报, 2025, 41(12): 100190 - .
[14]	魏勉, 程畅, 何博文, 程蓓, 戚克振, 别传彪. 无机-有机CdS/YBTPy S型光催化剂高效产氢及其机理[J]. 物理化学学报, 2025, 41(12): 100158 - .
[15]	雷嘉莉, 王娟, 张文慧, 王国宏, 梁子辉, 李金懋. TiO₂/CdIn₂S₄ S型异质结光催化剂促进光催化产氢耦合香兰醇氧化[J]. 物理化学学报, 2025, 41(12): 100174 - .

W₁₈O₄₉/铝掺杂SrTiO₃ S型异质结在LSPR效应辅助下实现全光谱太阳光驱动的光催化产氢

W₁₈O₄₉/Al-doped SrTiO₃ S-scheme heterojunction aided by the LSPR effect for full-spectrum solar light-driven photocatalytic hydrogen evolution

RichHTML

PDF

赞

补充材料