无机材料学报 ›› 2022, Vol. 37 ›› Issue (9): 1001-1008.DOI: 10.15541/jim20210806
陈瀚翔1(), 周敏1, 莫曌2, 宜坚坚3, 李华明2, 许晖2(
)
收稿日期:
2021-12-30
修回日期:
2022-04-27
出版日期:
2022-09-20
网络出版日期:
2022-05-09
通讯作者:
许 晖, 教授. E-mail: xh@ujs.edu.cn作者简介:
陈瀚翔(1993-), 男, 博士研究生. E-mail: 2350505633@qq.com
基金资助:
CHEN Hanxiang1(), ZHOU Min1, MO Zhao2, YI Jianjian3, LI Huaming2, XU Hui2(
)
Received:
2021-12-30
Revised:
2022-04-27
Published:
2022-09-20
Online:
2022-05-09
Contact:
XU Hui, professor. E-mail: xh@ujs.edu.cnAbout author:
CHEN Hanxiang (1993-), male, PhD candidate. E-mail: 2350505633@qq.com
Supported by:
摘要:
在光催化产氢反应中引入助催化剂可促进光生电子快速转移, 是提高光催化活性的有效方法。而目前, 高效助催化剂主要仍然是贵金属, 其高昂的价格极大限制了实际应用。本研究探讨了构筑非贵金属助催化剂CoN与g-C3N4 0D/2D紧密界面对光催化制氢性能的影响。负载非贵金属助催化剂CoN可以有效提高2D g-C3N4的光催化制氢活性, 负载量对其活性也有影响。构筑的0D/2D紧密界面有利于光生电子快速传输。两者的共同作用使得10% CoN/2D g-C3N4复合物光催化制氢效率达到403.6 μmol·g-1·h-1, 是2D g-C3N4单体的20倍。在CoN/2D g-C3N4复合材料中, 负载CoN作为析氢助催化剂可以显著促进电荷转移过程, 从而大幅提高光催化析氢活性。
中图分类号:
陈瀚翔, 周敏, 莫曌, 宜坚坚, 李华明, 许晖. CoN/g-C3N4 0D/2D复合结构及其光催化制氢性能研究[J]. 无机材料学报, 2022, 37(9): 1001-1008.
CHEN Hanxiang, ZHOU Min, MO Zhao, YI Jianjian, LI Huaming, XU Hui. 0D/2D CoN/g-C3N4 Composites: Structure and Photocatalytic Performance for Hydrogen Production[J]. Journal of Inorganic Materials, 2022, 37(9): 1001-1008.
图1 (a)2D g-C3N4, CoN/2D g-C3N4复合催化剂和CoN的XRD图谱, (b)2D g-C3N4和CoN/2D g-C3N4复合催化剂的FT-IR谱图, (c)2D g-C3N4, CoN/2D g-C3N4复合催化剂和CoN的紫外-可见光漫反射吸收光谱图, (d)2D g-C3N4和10% CoN/2D g-C3N4的氮气吸附-脱附等温线
Fig. 1 (a) XRD patterns of 2D g-C3N4, and 10% CoN/2D g-C3N4 samples, and CoN, (b) FT-IR spectra of 2D g-C3N4, and CoN/2D g-C3N4 samples, (c) UV-Vis diffuse reflectance spectra of 2D g-C3N4, and CoN/2D g-C3N4 samples, and CoN, (d) N2 adsorption-desorption isomers of 2D g-C3N4 and 10% CoN/2D g-C3N4 Colorful figures are available on website
图2 (a)2D g-C3N4, (b)CoN和(c)10% CoN/2D g-C3N4的SEM照片, 10% CoN/2D g-C3N4的(d, e)TEM照片和(f)高倍TEM照片
Fig. 2 SEM images of (a) 2D g-C3N4, (b) CoN and (c) 10% CoN/2D g-C3N4, and (d, e) TEM images and (f) HR-TEM image of 10% CoN/2D g-C3N4
图3 (a)2D g-C3N4和CoN/2D g-C3N4复合催化剂的光催化制氢速率测试, (b)10% CoN/2D g-C3N4复合催化剂的制氢稳定性测试(10% TEOA作为牺牲剂, 10 mg催化剂, 氙灯作为光源, λ>400 nm)
Fig. 3 (a) Photocatalytic hydrogen evolution with photocatalysts under visible light irradiation, and (b) hydrogen evolution stability test of 10% CoN/2D g-C3N4 under visible light irradiation (10% TEOA as sacrificial agent, 10 mg catalyst usage, xenon lamp as light source, λ>400 nm) Colorful figures are available on website
图4 2D g-C3N4和10% CoN/2D g-C3N4的(a)稳态荧光光谱图(激发波长为384 nm), (b)光电流响应图, (c)电化学阻抗谱图和(d)2D g-C3N4和10% CoN/2D g-C3N4的莫特肖特基曲线
Fig. 4 (a) Steady-state PL spectra excited at 384 nm, (b) photocurrent-time dependence, (c) electrochemical impedance spectra (EIS) of 2D g-C3N4 and 10% CoN/2D g-C3N4, and (d) Motschottky (MS) curves of 2D g-C3N4 and 10% CoN/2D g-C3N4 Colorful figures are available on website
图5 2D g-C3N4和10% CoN/2D g-C3N4在(a, b)可见光照射和(c, d)暗处的(a, c)超氧自由基和(b, d)羟基自由基ESR谱图
Fig. 5 ESR spectra of (a, c) DMPO-·O2- and (b, d) ·OH O2- and (b, d) ·OH (a, b) under visible-light irradiation and (c, d) without light irradiation of the 2D g-C3N4 and 10% CoN/2D g-C3N4 Colorful figures are available on website
Photocatalyst | Type of strategy | HER performance /(μmol·g-1·h-1) | Ref. |
---|---|---|---|
CoN/2D g-C3N4 | Nanosheets Nanostructure | 403.6 | This work |
Melem Oligomer | Functional group | 90 | [6] |
MoS2/g-C3N4 | Cocatalyst | 7.5 | [7] |
BP/g-C3N4 | Cocatalyst | 43 | [8] |
MoSe2/g-C3N4 | Cocatalyst | 7.5 | [9] |
p-n junction of g-C3N4 | Type II | 140 | [10] |
g-C3N4-NaI-WO3 | Z-scheme | 36 | [11] |
W18O49/g-C3N4 | Plasmonic effect | 4.8 | [12] |
表S1 不同类型g-C3N4的策略及其析氢性能
Table S1 Different types of strategies for g-C3N4 and their hydrogen evolution performance
Photocatalyst | Type of strategy | HER performance /(μmol·g-1·h-1) | Ref. |
---|---|---|---|
CoN/2D g-C3N4 | Nanosheets Nanostructure | 403.6 | This work |
Melem Oligomer | Functional group | 90 | [6] |
MoS2/g-C3N4 | Cocatalyst | 7.5 | [7] |
BP/g-C3N4 | Cocatalyst | 43 | [8] |
MoSe2/g-C3N4 | Cocatalyst | 7.5 | [9] |
p-n junction of g-C3N4 | Type II | 140 | [10] |
g-C3N4-NaI-WO3 | Z-scheme | 36 | [11] |
W18O49/g-C3N4 | Plasmonic effect | 4.8 | [12] |
图S1 (a)10% CoN/2D g-C3N4的SEM照片, (b~d)C、N、Co的EDS元素分布图
Fig. S1 (a) SEM image of 10% CoN/2D g-C3N4, (b-d) EDS elemental mappings from C, N and Co corresponding to 10% CoN/2D g-C3N4
图S2 (a)10% CoN/2D g-C3N4和2D g-C3N4的XPS全谱图, (b)CoN和10% CoN/2D g-C3N4的Co2p高分辨XPS图谱, 2D g-C3N4和10% CoN/2D g-C3N4的(c)C1s和(d)N1s高分辨XPS图谱
Fig. S2 (a) XPS survey spectra of 10% CoN/2D g-C3N4 and 2D g-C3N4, (b) Co2p XPS spectra of CoN and 10% CoN/2D g-C3N4, (c) C1s and (d) N1s XPS spectra of 2D g-C3N4 and 10% CoN/2D g-C3N4
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