构筑先进二维异质结构Ag/WO3−x用于提升光电转化效率

doi:10.3866/PKU.WHXB201812054

摘要/Abstract

摘要：

等离子体激元诱导的光电化学反应被认为是太阳能转换的有效的替代方案。寻找具有增强的光吸收以及更长载流子寿命的高效光催化剂对于提高太阳能的转换效率至关重要，但其制备却具有挑战性。我们制备了Ag纳米颗粒均匀负载的二维(2D)无定形三氧化钨(a-WO_3−x)，并对其进行退火处理，所获得的纳米异质结用作光电极材料具有高效的光电转化效率，并且其光氧化降解性能也显著提升。该光电阳极的高光电催化(PEC)性能归因于等离子体金属Ag纳米颗粒的局部表面等离子共振(LSPR)效应能够增强体系的光吸收和热电子转移。此外，局部结晶-非晶界面的构筑可以进一步提高光生电子-空穴对的分离效率并增加体系的导电性。

10.3866/PKU.WHXB201809013.F009

关键词: 二维材料, 等离子体金属/半导体异质结构, PEC转换

Abstract:

Solar energy, which is clean, affordable and reliable, can help alleviate the current environmental pollution and energy crisis efficiently. In the past few decades, great progress has been made in harvesting and converting solar energy into chemical energy. Among various technologies, plasmon-induced photoelectrochemistry has been proposed as a promising alternative for solar energy conversion. The hot electrons generated from plasmon excitation and transfer from metal nanostructures to semiconductors is a potential new paradigm for solar energy conversion. However, the ultrafast decay of the hot carriers is unfavorable for the improvement of photocatalytic efficiency. Therefore, finding more efficient photocatalysts, with enhanced light absorption and a longer carrier lifetime, is of paramount importance for improving the conversion efficiency of solar energy, but their fabrication is challenging. In this work, a plasmonic metal/semiconductor heterostructure based on Ag nanoparticles embedded in two-dimensional (2D) amorphous sub-stoichiometric tungsten trioxide (a-WO_3−x), followed by annealing, was successfully fabricated. Firstly, the peculiar nanostructure of 2D a-WO_3−x was successfully constructed from WS₂ nanosheets with supercritical CO₂ (SC CO₂) at 200 ℃. Secondly, the Ag/a-WO_3−x heterostructure was synthesized using an in situ reduction method. Finally, the obtained 2D heterostructure of Ag/WO_3−x was annealed at 400 ℃ in N₂ to further improve its stability and conductivity. X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) were used to characterize the structure, morphology, and composition of the material, respectively. UV-Vis spectra were also measured to evaluate light adsorption. Characterization results show that the amorphous structure can effectively anchor metal nanoparticles, and the metal nanoparticles are uniformly dispersed in the amorphous region and have a small size. The as-prepared nanocomposites showed efficient photoelectrochemical (PEC) water splitting when serving as photoelectrode materials, and efficient PEC activity towards photo-oxidation degradation currents under excitation of Ag localized surface plasmon resonance (LSPR). The photocurrent response of the Ag/WO_3−x heterostructure was approximately five times greater than that of a-WO_3−x. Moreover, the PEC degradation efficiency of Ag/WO_3−x reached 96.7% for MO under Vis light illumination (after reaction for 120 min), while the PEC degradation efficiency of WO_3−x was only 63.6%. The high PEC performance of the composite photoanode can be ascribed to the local surface plasmon resonance (LSPR) effect of the Ag nanoparticles, which can enhance the light absorption and hot electron transformation. Moreover, the construction of local crystalline-amorphous interfaces can further promote the separation efficiency of the photogenerated electron-hole pairs, and thus increase conductivity. This work provides a positive strategy for the fabrication of advanced photocatalysts, and a new perspective on understanding of the synergistic effects of structural and electronic regulations.

Key words: Two-dimensional material, Plasmonic metal/semiconductor heterostructure, PEC conversion

任玉美,许群. 构筑先进二维异质结构Ag/WO₃₋_x用于提升光电转化效率[J]. 物理化学学报, 2019, 35(10): 1157-1164.

Yumei REN,Qun XU. Construction of Advanced Two-dimensional Heterostructure Ag/WO_3−x for Enhancing Photoelectrochemical Performance[J]. Acta Physico-Chimica Sinica, 2019, 35(10): 1157-1164.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201812054

https://www.whxb.pku.edu.cn/CN/Y2019/V35/I10/1157

图/表 7

Scheme 1

Fig 1

Fig 2

Fig 3

Fig 4

Fig 5

Fig 6

参考文献 45

1	Wang F. F. ; Li Q. ; Xu D. S. Adv. Energy Mater. 2017, 7 (23), 1700529. doi: 10.1002/aenm.201700529
2	Wu N. Q. Nanoscale 2018, 10, 2679. doi: 10.1039/C7NR08487K
3	Walter M. G. ; Warren E. L. ; McKone J. R. ; Boettcher S. W. ; Mi Q. ; Santori E. A. ; Lewis N. S. Chem. Rev. 2010, 110 (11), 6446. doi: 10.1021/cr1002326
4	Li J. T. ; Wu N. Q. Catal. Sci. Tech. 2015, 5, 1360. doi: 10.1039/C4CY00974F
5	Xia H. C. ; Xu Q. ; Zhang J. N. Nano Micro Lett. 2018, 10 (4), 66. doi: 10.1007/s40820-018-0219-z
6	Chen X. B. ; Shen S. H. ; Guo L. J. ; Mao S. S. Chem. Rev. 2010, 110 (11), 6503. doi: 10.1021/cr1001645
7	Vuong N. M. ; Kim D. ; Kim H. Sci. Rep. 2015, 5, 11040. doi: 10.1038/srep11040
8	Kong Y. Q. ; Sun H. G. ; Fan W. L. ; Wang L. ; Zhao H. K. ; Zhao X. ; Yuan S. Z. RSC Adv. 2017, 7, 15201. doi: 10.1039/c7ra01426k
9	Ling C. Y. ; Wang J. L. Acta Phys.-Chim. Sin. 2017, 33 (5), 869. doi: 10.3866/PKU.WHXB201702088
	凌崇益; 王金兰. 物理化学学报, 2017, 33 (5), 869. doi: 10.3866/PKU.WHXB201702088
10	Shang Y. ; Chen Y. ; Shi Z. B. ; Zhang D. F. ; Guo L. Acta Phys.-Chim. Sin. 2013, 29 (8), 1819. doi: 10.3866/PKU.WHXB201305281
	商旸; 陈阳; 施湛斌; 张东凤; 郭林. 物理化学学报, 2013, 29 (8), 1819. doi: 10.3866/PKU.WHXB201305281
11	Cushing S. K. ; Wu N. J. Phys. Chem. Lett. 2016, 7 (4), 666. doi: 10.1021/acs.jpclett.5b02393
12	Zhang Y. C. ; He S. ; Guo W. X. ; Hu Y. ; Huang J. W. ; Mulcahy J. R. ; Wei W. D. Chem. Rev. 2018, 118 (6), 2927. doi: 10.1021/acs.chemrev.7b00430
13	Clavero C. Nat. Photonics 2014, 8, 95. doi: 10.1038/NPHOTON.2013.238
14	Tian Y. ; Tatsuma T. J. Am. Chem. Soc. 2005, 127 (20), 7632. doi: 10.1021/ja042192u
15	Naseri N. ; Qorbani M. ; Kim H. ; Choi W. ; Moshfegh A. Z. J. Phys. Chem. C 2015, 119 (3), 1271. doi: 10.1021/jp507988c
16	Du X. H. ; L. Y. ; Y. H. ; Xiang Q. J. Acta Phys.-Chim. Sin. 2018, 34 (4), 414. doi: 10.3866/PKU.WHXB201708283
	杜新华; 李阳;殷辉;向全军. 物理化学学报, 2018, 34 (4), 414. doi: 10.3866/PKU.WHXB201708283
17	Nie L. H. ; Hu Y. ; Zhang W. X. Acta Phys.-Chim. Sin. 2012, 28 (1), 154. doi: 10.3866/PKU.WHXB201228154
	聂龙辉; 胡瑶; 张旺喜. 物理化学学报, 2012, 28 (1), 154. doi: 10.3866/PKU.WHXB201228154
18	Xia H. C. ; Zhang J. N. ; Chen Z. M. ; Xu Q. Appl. Surf. Sci. 2018, 440, 91. doi: 10.1016/j.apsusc.2017.12.263
19	Xia H. C. ; Zhang J. N. ; Yang Z. ; Guo S. Y. ; Guo S. H. ; Xu Q. Nano Micro Lett. 2017, 9 (4), 43. doi: 10.1007/s40820-017-0144-6
20	Tian Y. ; Tatsuma T. Chem. Commun. 2004, 1810. doi: 10.1039/B405061D
21	Tian Y. ; Tatsuma T. J. Am. Chem. Soc. 2005, 127 (20), 7632. doi: 10.1021/ja042192u
22	Lee S. H. ; Lee S. W. ; Oh T. ; Petrosko S. H. ; Mirkin C. A. ; Jang J. W. Nano Lett. 2018, 18 (1), 109. doi: 10.1021/acs.nanolett.7b03540
23	Li J. ; Cushing S. K. ; Chu D. ; Zheng P. ; Bright J. ; Castle C. ; Manivannan A. ; Wu N. J. Mater. Res. 2016, 31 (11), 1608. doi: 10.1557/jmr.2016.102
24	Ren Y. M. ; Li C. ; Xu Q. ; Yan J. ; Li Y. Z. ; Yuan P. F. ; Xia H. C. ; Niu C. Y. ; Yang X. A. ; Jia Y. Appl. Catal. B: Environ. 2019, 245, 648. doi: 10.1016/j.apcatb.2019.01.015
25	Ren Y. M. ; Xu Q. Energ. Environ. Mater. 2018, 1 (2), 46. doi: 10.1016/j.apcatb.2019.01.015
26	Ren Y. M. ; Wang C. Z. ; Qi Y. H. ; Chen Z. M. ; Jia Y. ; Xu Q. Appl. Surf. Sci. 2017, 419, 573. doi: 10.1016/j.apsusc.2017.05.058
27	Wang N. ; Xu Q. ; Xu S. S. ; Qi Y. H. ; Chen M. ; Li H. X. ; Han B. X. Sci. Rep. 2015, 5, 16764. doi: 10.1038/srep16764
28	Ren Y. M. ; Xu Q. ; Zheng X. L. ; Fu Y. Z. ; Wang Z. ; Chen H. L. ; Weng Y. X. ; Zhou Y. C. Appl. Catal. B: Environ. 2018, 231, 381. doi: 10.1016/j.apcatb.2018.03.040
29	Wang Y. L. ; Cui X. B. ; Yang Q. Y. ; Liu J. ; Gao Y. ; Sun P. ; Lu G. Y. Sensor. Actuat. B 2016, 225, 544. doi: 10.1016/j.snb.2015.11.065
30	Chen F. ; Yang Q. ; Li X. M. ; Zeng G. M. ; Wang D. B. ; Niu C. G. ; Zhao J. W. ; An H. X. ; Xie T. ; Deng Y. C. Appl. Catal. B: Environ. 2017, 200, 330. doi: 10.1016/j.apcatb.2016.07.021
31	Shi Y. ; Wang J. ; Wang C. ; Zhai T. T. ; Bao W. J. ; Xu J. J. ; Xia X. H. ; Chen H. Y. J. Am. Chem. Soc. 2015, 137 (23), 7365. doi: 10.1021/jacs.5b01732
32	Zafra M. C. ; Lavela P. ; Rasines G. ; Macías C. ; Tirado J. L. ; Ania C. O. Electrochim. Acta 2014, 135, 208. doi: 10.1016/j.electacta.2014.04.182
33	Lewera A. ; Timperman L. ; Roguska A. ; Alonso-Vante N. J. Phys. Chem. C 2011, 115 (41), 20153. doi: 10.1021/jp2068446
34	Yin L. ; Chen D. L. ; Feng M. J. ; Ge L. F. ; Yang D. W. ; Song Z. H. ; Fan B. B. ; Zhang R. ; Shao G. S. RSC Adv. 2015, 5, 328. doi: 10.1039/c4ra10500a
35	Cheng H. F. ; Huang B. B ; Wang P. ; Wang Z. Y. ; Lou Z. Z. ; Wang J. P. ; Qin X. Y. ; Zhang X. Y. ; Dai Y. Chem. Commun 2011, 47, 7054. doi: 10.1039/c1cc11525a
36	Dong P. Y. ; Yang B. R. ; Liu C. ; Xu F. H. ; Xi X. G. ; Hou G. H. ; Shao R. RSC Adv. 2017, 7, 947. doi: 10.1039/c6ra25272a
37	Miyauchi M. Phys. Chem. Chem. Phys. 2008, 10, 6258. doi: 10.1039/b807426g
38	Wang Q. ; Moser J. E. ; Gra1tzel M. J. Phys. Chem. B 2005, 109 (31), 14945. doi: 10.1021/jp052768h
39	Chen X. Q. ; Li P. ; Tong H. ; Kako T. ; Ye J. H. Sci. Technol. Adv. Mater. 2011, 12, 044604. doi: 10.1088/1468-6996/12/4/044604
40	Pu Y. C. ; Wang G. M. ; Chang K. D. ; Ling Y. C. ; Lin Y. K. ; Fitzmorris B. C. ; Liu C. M. ; Lu X. L. ; Tong Y. X. ; Zhang J. Z. ; et al Nano Lett. 2013, 13 (8), 3817. doi: 10.1021/nl4018385
41	Robatjazi H. ; Bahauddin S. M. ; Doiron C. ; Thomann I. Nano Lett. 2015, 15 (9), 6155. doi: 10.1021/acs.nanolett.5b02453
42	Xu F. ; Yao Y. W. ; Bai D. D. ; Xu R. S. ; Mei J. J. ; Wu D. P. ; Gao Z. Y. ; Jiang K. RSC Adv. 2015, 5, 60339. doi: 10.1039/c5ra06241a
43	Hisatomi T. ; Kubota J. ; Domen K. Chem. Soc. Rev. 2014, 43, 7520. doi: 10.1039/c3cs60378d
44	Chen H. R. ; Shen K. ; Chen J. Y. ; Chen X. D. ; Li Y. E. J. Mater. Chem. A 2017, 5, 9937. doi: 10.1039/c7ta02184d
45	Li D. ; Xing Z. P. ; Yu X. J. ; Cheng X. W. Electrochim. Acta 2015, 170, 182. doi: 10.1016/j.electacta.2015.04.148

[1]	曹晓辉, 侯成义, 李耀刚, 李克睿, 张青红, 王宏志. 基于MXenes的功能纤维的制备及其在智能可穿戴领域的应用[J]. 物理化学学报, 2022, 38(9): 2204058 - .
[2]	阙海峰, 江华宁, 王兴国, 翟朋博, 孟令佳, 张鹏, 宫勇吉. 二维材料范德华间隙的利用[J]. 物理化学学报, 2021, 37(11): 2010051 - .
[3]	王易,霍旺晨,袁小亚,张育新. 二氧化锰与二维材料复合应用于超级电容器[J]. 物理化学学报, 2020, 36(2): 1904007 - .
[4]	谭淼,张磊,梁万珍. 基于二维材料WX₂构建的范德华异质结的结构和性质及应变效应的理论研究[J]. 物理化学学报, 2019, 35(4): 385 -393 .
[5]	杜春保,胡小玲,张刚,程渊. 二维材料“遇见”生物大分子：机遇与挑战[J]. 物理化学学报, 2019, 35(10): 1078 -1089 .
[6]	李家意,丁一,张卫,周鹏. 基于二维材料及其范德瓦尔斯异质结的光电探测器[J]. 物理化学学报, 2019, 35(10): 1058 -1077 .
[7]	程龙,刘公平,金万勤. 二维材料膜在气体分离领域的最新研究进展[J]. 物理化学学报, 2019, 35(10): 1090 -1098 .
[8]	陈熙,张胜利. 基于3d元素掺杂的石墨二炔分子传感材料性能调控[J]. 物理化学学报, 2018, 34(9): 1061 -1073 .
[9]	凌崇益,王金兰. 基于类石墨烯二维材料的析氢反应电催化剂的研究进展[J]. 物理化学学报, 2017, 33(5): 869 -885 .
[10]	贺雷,张向倩,陆安慧. 二维炭基多孔材料的合成及应用[J]. 物理化学学报, 2017, 33(4): 709 -728 .
[11]	曾梦琪,张涛,谭丽芳,付磊. 液态金属催化剂:二维材料的点金石[J]. 物理化学学报, 2017, 33(3): 464 -475 .
[12]	张绍政,刘佳,谢燕,陆银稷,李林,吕亮,杨建辉,韦世豪. 二维M₂XO_2-2x(OH)_2x(M=Ti, V;X=C, N)析氢催化活性的第一性原理研究[J]. 物理化学学报, 2017, 33(10): 2022 -2028 .
[13]	石乃恩,宋传远,张俊,黄维. 金属卟啉二维纳米晶的制备及其光电性能[J]. 物理化学学报, 2016, 32(10): 2447 -2461 .
[14]	杨建辉, 计嘉琳, 李林, 韦世豪. 二维TiC 层表面H₂的化学吸附与物理吸附[J]. 物理化学学报, 2014, 30(10): 1821 -1826 .

构筑先进二维异质结构Ag/WO₃₋_x用于提升光电转化效率

Construction of Advanced Two-dimensional Heterostructure Ag/WO_3−x for Enhancing Photoelectrochemical Performance

RichHTML

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

图/表 7

参考文献 45

相关文章 14

Metrics

推荐阅读 0