通过直接S型电荷转移和高度改进的可见光驱动光催化效率构建3D花状O-掺杂g-C3N4-[N-掺杂Nb2O5/C]异质结

doi:10.1016/S1872-2067(21)64038-X

催化学报 ›› 2022, Vol. 43 ›› Issue (10): 2637-2651.DOI: 10.1016/S1872-2067(21)64038-X

通过直接S型电荷转移和高度改进的可见光驱动光催化效率构建3D花状O-掺杂g-C₃N₄-[N-掺杂Nb₂O₅/C]异质结

Fahim A. Qaraah^a, Samah A. Mahyoub^b, Abdo Hezam^c, Amjad Qaraah^d, Qasem A. Drmosh^e, 修光利^a^,^*()

^a华东理工大学资源与环境工程学院, 国家环境保护化工过程环境风险评估与控制重点实验室, 上海 200237, 中国
^b华东理工大学化学工程学院, 化学工程国家重点实验室, 上海 200237, 中国
^c莱布尼茨-罗斯托克大学催化研究所, 罗斯托克, 德国
^d天津大学化学工程与技术学院, 天津 300350, 中国
^e法赫德国王石油与矿业大学(KFUPM)氢与储能交叉学科研究中心(IRC-HES), 沙特阿拉伯

收稿日期:2022-01-28 接受日期:2022-02-15 出版日期:2022-10-18 发布日期:2022-09-30
通讯作者: 修光利
基金资助:
上海市科委资助(19DZ1205001);上海市生态环境局拨款(沪环科[2021]-46)

Construction of 3D flowers-like O-doped g-C₃N₄-[N-doped Nb₂O₅/C] heterostructure with direct S-scheme charge transport and highly improved visible-light-driven photocatalytic efficiency

Fahim A. Qaraah^a, Samah A. Mahyoub^b, Abdo Hezam^c, Amjad Qaraah^d, Qasem A. Drmosh^e, Guangli Xiu^a^,^*()

^aState Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Processes, School of Resources & Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China
^bState Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
^cLeibniz-Institute for Catalysis at the University of Rostock, 18059 Rostock, Germany
^dSchool of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
^eInterdisciplinary Research Center for Hydrogen and Energy Storage (IRC-HES), King Fahd University of Petroleum & Minerals (KFUPM), Dhahran 31261, Saudi Arabia

Received:2022-01-28 Accepted:2022-02-15 Online:2022-10-18 Published:2022-09-30
Contact: Guangli Xiu
Supported by:
Science and Technology Commission of Shanghai Municipality(19DZ1205001);Shanghai Municipal Bureau of Ecology and Environment Grant(huhuanke [2021]-46)

摘要/Abstract

摘要：

通过将两种光催化材料复合构建合适的异质结构光催化体系, 可设计出广泛应用于环境、医疗和能源领域的高效光催化剂. 近年来, S型异质结体系因可实现高效的光生载流子分离, 同时表现出较强的光氧化还原能力而备受关注.

本文通过超声和剧烈搅拌的方法构建了由2D O-掺杂g-C₃N₄(OCN)纳米片和3D N-掺杂Nb₂O₅/C(N-NBO/C)纳米花组成的新型S型异质结体系, 经过热处理后用于罗丹明B(RhB)的光催化降解. 实验结果表明, 优化的4OCN-[N-NBO/C] (OCN和N-NBO/C含量分别为40 mg和100 mg)样品表现出较好的理化特性, 其比表面积大、载流子的分离效率高、可见光吸收效率大和紧邻接触面大. EPR试验和自由基捕获实验结果表明, OCN和N-NBO/C之间形成了S型异质结. RhB光催化降解实验结果表明, 在可见光照射下, 所制备的材料表现出较好的催化性能, 催化剂光催化效率高, 稳定性好. 光催化降解性能的提高可归因于快速电荷转移、高效电荷分离、光致电荷载流子的寿命延长以及S型体系中光致电荷的高氧化还原能力. 本文还深入研究了催化剂的组成、结构、形貌以及RhB的光催化降解机制, 为相关研究提供了一定参考.

关键词: 2D/3D纳米结构, S型异质结, g-C₃N₄, Nb₂O₅, 光催化降解

Abstract:

Constructing a suitable heterojunction photocatalytic system from two photocatalytic materials is an efficient approach for designing extremely efficient photocatalysts for a broader range of environmental, medical, and energy applications. Recently, the construction of a step-scheme heterostructure system (hereafter called the S-scheme) has received widespread attention in the photocatalytic field due to its ability to achieve efficient photogenerated carrier separation and obtain strong photo-redox ability. Herein, a novel S-scheme heterojunction system consisting of 2D O-doped g-C₃N₄ (OCN) nanosheets and 3D N-doped Nb₂O₅/C (N-NBO/C) nanoflowers is constructed via ultrasonication and vigorous agitation technique followed by heat treatment for the photocatalytic degradation of Rhodamine B (RhB). Detailed characterization and decomposition behaviour of RhB showed that the fabricated material shows excellent photocatalytic efficiency and stability towards RhB photodegradation under visible-light illumination. The enhanced performance could be attributed to the following factors: fast charge transfer, highly-efficient charge separation, extended lifetime of photoinduced charge carriers, and the high redox capability of the photoinduced charges in the S-scheme system. Various trapping experiment conditions and electron paramagnetic resonance provide clear evidence of the S-scheme photogenerated charge transfer path, meanwhile, the RhB mineralization degradation pathway was also investigated using LC-MS. This study presents an approach to constructing Nb₂O₅-based S-scheme heterojunctions for photocatalytic applications.

Key words: 2D/3D nanostructure, S-scheme heterojunction, g-C₃N₄, Nb₂O₅, Photocatalytic degradation

Fahim A. Qaraah, Samah A. Mahyoub, Abdo Hezam, Amjad Qaraah, Qasem A. Drmosh, 修光利. 通过直接S型电荷转移和高度改进的可见光驱动光催化效率构建3D花状O-掺杂g-C₃N₄-[N-掺杂Nb₂O₅/C]异质结[J]. 催化学报, 2022, 43(10): 2637-2651.

Fahim A. Qaraah, Samah A. Mahyoub, Abdo Hezam, Amjad Qaraah, Qasem A. Drmosh, Guangli Xiu. Construction of 3D flowers-like O-doped g-C₃N₄-[N-doped Nb₂O₅/C] heterostructure with direct S-scheme charge transport and highly improved visible-light-driven photocatalytic efficiency[J]. Chinese Journal of Catalysis, 2022, 43(10): 2637-2651.

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图/表 12

Scheme 1. Formation pathway of 3D S-scheme OCN-[N-NBO/C] heterostructure.

Fig. 1. XRD patterns (a) and FT-IR spectra (b) of the as-fabricated OCN, N-NBO/C, 1OCN-[N-NBO/C], 4OCN-[N-NBO/C] and 8OCN-[N-NBO/C].

Fig. 2. SEM images of OCN nanosheet (a), N-NBO/C nanoflowers (b), and representative and magnified SEM images of the S-scheme 4OCN-[N-NBO/C] heterostructures (c,d). TEM images of as-prepared OCN (e), N-NBO/C (f) and 4OCN-[N-NBO/C] (g). Parallel TEM-EDX mapping images of C (h), Nb (i), O (j), and N (k) of the 4OCN-[N-NBO/C] heterostructures, and HRTEM image of the S-scheme 4OCN-[N-NBO/C] heterostructures (l).

Fig. 3. (a) N2 adsorption-desorption isotherms of the OCN, N-NBO/C, 1OCN-[N-NBO/C], 4OCN-[N-NBO/C], 8OCN-[N-NBO/C] (a), and the related pore size distribution curves (b).

Fig. 4. (a) UV-vis diffused reflectance of Pure CN, OCN, Pure Nb2O5, N-NBO/C, and OCN-[N-NBO/C ] composites. (b) Tauc plots of Pure CN, OCN, Pure Nb2O5, N-NBO/C. (c,d) MS plots for N-NBO/C and OCN.

Fig. 5. High-resolution XPS spectra of C 1s (a), N 1s (b), O 1s (c), and Nb 3d (d) of the OCN, N-NBO/C, and 4OCN-[N-NBO/C] samples.

Fig. 6. The change in concentration of RhB vs. illumination time over OCN, N-NBO/C, and xOCN-[N-NBO/C] composites (a), the kinetic curves of RhB degradation with numerous photocatalysts under visible light illumination as a pseudo-first-order reaction (b,c). (d) Cycling experiments of photodegradation RhB over OCN-[N-NBO/C]. XRD (e) and FTIR (f) of OCN-[N-NBO/C] before and after photocatalysis.

Table 1 Summarizes the photodegradation performance of RhB under visible light by using various heterojunction photocatalysts.

Photocatalyst	Morphology	Heterojunction type	RhB Conc. (mg/L)	Catalyst Conc. (mg/L)	Visible light source	k (min^-1)	Time (min)	Ref.
g-C₃N₄/Nb₂O₅	nanofibers	type-II	10	500	300 W XL	0.0363	120	[51]
g-C₃N₄/Nb₂O₅	nanoparticles	type-II	10	500	15 W	0.0202	90	[52]
g-C₃N₄/Nb₂O₅/rGA	nanocomposites	heterojunction	20	300	300W XL	—	100	[53]
CeO₂/NaNbO₃	—	heterojunction	10	400	300 W Hg lamp	0.073	30	[54]
mpg-C₃N₄/Bi₂WO₆	—	—	50	500	300 W XL	0.0724	60	[55]
g-C₃N₄/TiO₂/CuO	nanocomposites	S-scheme	50	500	500 W XL	0.00916	120	[56]
BiOBr/g-C₃N₄	—	S-scheme	10	300	300W XL	0.01274	30	[57]
MoO₃/Bi₂O₄	—	Z-scheme	10	500	100 W LED	—	40	[58]
TiO₂/WS₂	microspheres	heterojunction	20	200	300W XL	0.0371	90	[59]
g-C₃N₄@C-TiO₂	microstructures	Z-scheme	10	1000	350W XL	0.036	90	[60]
OCN-[N-NBO/C]	nanoflowers	S-scheme	40	100	300 W XL	0.1477	30	Reporting

Fig. 7. (a) RhB degradation at different pH values. (b) RhB adsorption at different pH levels. (c) Different catalytic dosages over 4OCN-[N-NBO/C]. (d) RhB degradation at different concentrations.

Fig. 8. Photocurrent transient curves (a) and EIS (b) of OCN, N-NBO/C, and 4OCN-[N-NBO/C]; PL spectra (c), time-resolved fluorescence spectra (d), and photocatalytic degradation (e) of RhB by 4OCN-[N-NBO/C] under varied trapping experiment circumstances. (f) Schematic diagrams of conventional S-scheme heterojunction.

Fig. 9. EPR spectra of DMPO-•OH adducts (in water solution) (a) and DMPO-•O2- adducts (in methanol solution) (b) over N-NBO/C, OCN, and 4OCN-[N-NBO/C] under irradiation for 3 min. (c) Schematic elucidation of the S-scheme transfer mechanism between OCN and N-NBO/C: (i) before contact, (ii) after contact, and (iii) after contact under illumination.

Fig. 10. Possible photocatalytic degradation pathways of RhB.

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通过直接S型电荷转移和高度改进的可见光驱动光催化效率构建3D花状O-掺杂g-C₃N₄-[N-掺杂Nb₂O₅/C]异质结

Construction of 3D flowers-like O-doped g-C₃N₄-[N-doped Nb₂O₅/C] heterostructure with direct S-scheme charge transport and highly improved visible-light-driven photocatalytic efficiency

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[1]	赵彬彬, 钟威, 陈峰, 王苹, 别传彪, 余火根. 高晶化g-C₃N₄光催化剂: 合成、结构调控和光催化产氢[J]. 催化学报, 2023, 52(9): 127-143.
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[4]	宋明明, 宋相海, 刘鑫, 周伟强, 霍鹏伟. ZnIn₂S₄/MOF-808微球结构S型异质结光催化剂的制备及其光还原CO₂性能研究[J]. 催化学报, 2023, 51(8): 180-192.
[5]	李世杰, 王春春, 董珂欣, 张鹏, 陈晓波, 李鑫. 新型MIL-101(Fe)/BiOBr S型异质催化剂用于高效光催化降解抗生素和还原六价铬: 光催化性能分析和光催化机理研究[J]. 催化学报, 2023, 51(8): 101-112.
[6]	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(5): 267-278.
[7]	李宁, 高雪云, 苏俊珲, 高旸钦, 戈磊. 类金属WO₂/g-C₃N₄复合光催化剂的构造及其优异的光催化性能[J]. 催化学报, 2023, 47(4): 161-170.
[8]	Eun Hyup Kim, Min Hee Lee, Jeehye Kim, Eun Cheol Ra, Ju Hyeong Lee, Jae Sung Lee. 无碱CO₂加氢高效制甲酸Pd/g-C₃N₄催化剂的单原子和纳米簇的协同作用[J]. 催化学报, 2023, 47(4): 214-221.
[9]	李钱, 唐麒君, 熊珮瑶, 陈东之, 陈建孟, 吴忠标, 王海强. 钯化学态对g-C₃N₄光催化还原CO₂的影响: 单原子态在促进CH₄生成中的独特作用[J]. 催化学报, 2023, 46(3): 177-190.
[10]	李瀚, 陶善仁, 万思杰, 邱国根, 龙庆, 余家国, 曹少文. ZnCdS纳米球和二苯并噻吩修饰的g-C₃N₄构成的S型异质结用于增强光催化产氢[J]. 催化学报, 2023, 46(3): 167-176.
[11]	张志洁, 王雪盛, 唐慧玲, 李德本, 徐家跃. 调控Cs₃Bi₂Br₉@V_O-In₂O₃ S型异质结的费米能级和内建电场促进光生电荷分离和二氧化碳还原[J]. 催化学报, 2023, 55(12): 227-240.
[12]	吴优, 杨祎, 谷苗莉, 别传彪, 谭海燕, 程蓓, 许景三. 用于改进H₂O₂制备的1D/0D异质结的ZnIn₂S₄@ZnO S型光催化剂[J]. 催化学报, 2023, 53(10): 123-133.
[13]	林波, 夏梦阳, 许堡荣, 种奔, 陈子浩, 杨贵东. 仿生纳米结构的g-C₃N₄基光催化剂研究进展[J]. 催化学报, 2022, 43(8): 2141-2172.
[14]	雷洋, 黄剑锋, 李鑫奥, 吕楚滢, 侯超苹, 刘军民. 直接Z-scheme光催化复合体系: 金属有机卟啉笼负载于g-C₃N₄中以增强光解水产氢活性[J]. 催化学报, 2022, 43(8): 2249-2258.
[15]	苏凯艺, 张超锋, 王业红, 张健, 郭强, 高著衍, 王峰. 利用N-羟基邻苯二甲酰亚胺研究可见光照射下Nb₂O₅中高度扭曲的NbO₆单元作为电子转移位点[J]. 催化学报, 2022, 43(7): 1894-1905.