S-型Ag2S/Co1-xS@Co9S8@C纳米催化剂用于多光谱太阳能驱动降解持久性有机污染物左氧氟沙星

doi:10.1016/S1872-2067(26)65179-0

催化学报 ›› 2026, Vol. 89: 310-325.DOI: 10.1016/S1872-2067(26)65179-0

S-型Ag₂S/Co_1-_xS@Co₉S₈@C纳米催化剂用于多光谱太阳能驱动降解持久性有机污染物左氧氟沙星

Sangeeta Adhikari^a^,^b^,^c^,¹, Sandip Mandal^d^,^e^,¹, Do-Heyoung Kim^a^,^f^,^*

^a全南国立大学化学工程学院,光州,韩国
^b全南国立大学催化研究所,光州,韩国
^c维洛尔理工学院安得拉邦校区高等科学学院化学系,安得拉邦阿马拉瓦蒂,印度
^d朝鲜大学牙科学院,光州,韩国
^e朝鲜大学口腔软组织疾病治疗融合研究中心,光州,韩国
^f朱拉隆功大学工程学院化学工程系,曼谷,泰国

收稿日期:2026-01-18 接受日期:2026-04-16 出版日期:2026-10-18 发布日期:2026-09-01
通讯作者: *电子信箱: email-kdhh@chonnam.ac.kr (D.-H. Kim).
作者简介:
¹共同第一作者.

Multispectral solar-driven detoxification by S-scheme Ag₂S/Co_1-xS@Co₉S₈@C nanocatalyst of emerging persistent organic pollutant-levofloxacin

Sangeeta Adhikari^a^,^b^,^c^,¹, Sandip Mandal^d^,^e^,¹, Do-Heyoung Kim^a^,^f^,^*

^aSchool of Chemical Engineering, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186, Republic of Korea
^bCatalysis Research Institute, Chonnam National University, 77 Yongbong-ro, Buk-gu,Gwangju 61186, Republic of Korea
^cDepartment of Chemistry, School of Advanced Sciences, VIT-AP University, Beside AP Secretariat, Amaravati 522241, Andhra Pradesh, India
^dCollege of Dentistry, Chosun University, 7 Chosundaegil, Dong-gu, Gwangju 61452, Republic of Korea
^eConvergence Research Center for Treatment of Oral Soft Tissue Disease (MRC), Chosun University, 7 Chosundaegil, Dong-gu, Gwangju 61452, Republic of Korea
^fDepartment of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok 10330, Thailand

Received:2026-01-18 Accepted:2026-04-16 Online:2026-10-18 Published:2026-09-01
Contact: *E-mail: email-kdhh@chonnam.ac.kr (D.-H. Kim).
About author:
¹ Contributed equally to this work.

摘要/Abstract

摘要：

光生载流子的精准调控以及全太阳光谱的高效利用是提升光催化降解性能的核心技术路径. 构建S型异质结可依靠界面内建电场实现光生电子-空穴空间有效分离, 同时保留两端材料强氧化还原电位, 克服传统单一半导体载流子快速复合、光谱响应区间狭窄的固有缺陷. 本文合成了S-型Ag₂S/Co_1-_xS@Co₉S₈@C (A-CCC)异质结纳米催化剂; 强界面内建电场赋予该催化剂在紫外-近红外全波段模拟太阳光下优异的光催化降解性能. 扫描电镜、高分辨透射电镜、X-射线衍射、拉曼光谱和原位X-射线光电子能谱结果表明, Co-ZIF-67衍生的八面体形态与均匀分布的Ag₂S纳米粒子均得到很好保持, 形成不同的Co_1-_xS和Co₉S₈物相嵌入到碳基质中. 紫外光电子能谱和带隙测量阐明了由内部电场驱动的S-型异质结配置, 促进了界面电荷高效分离与迁移. 透射模式稳态太赫兹时域光谱、多指数拟合时间分辨光致发光谱及计算得到的振幅/强度加权平均载流子寿命(~2.38 ns)结果表明, 5 wt% 的Ag₂S CCC (5A-CCC)样品具备显著的界面电荷分离效应. 5A-CCC纳米催化剂对环境难降解抗生素左氧氟沙星(LCN)表现出优异光催化活性, 40 min内LCN降解率约99.7%, 表观速率常数为0.0326 min^-1. 该优异性能源于催化剂光谱吸收拓展至近红外波段, 可实现13.6%的高效光热转换, 与光催化过程形成协同效应. 自由基捕获实验与活性氧探针表征证实, 超氧自由基O₂^•-为左氧氟沙星降解的主导活性物种. 利用液相色谱-质谱联用观察到LCN降解的中间产物.

综上, 本文制备的Ag₂S/Co_1-_xS@Co₉S₈@C纳米催化体系具备优异的光催化性能, 为开发全光谱响应纳米催化剂、实现水体持久性抗生素环境修复提供理论依据与实验思路.

关键词: 持久性有机污染物, 左氧氟沙星, 全太阳光谱, S-型异质结, 界面电荷转移

Abstract:

Strategic regulation of photogenerated carriers along with efficient utilization of full solar spectrum is a crucial approach in photocatalytic reactions. In this aspect, creating S-scheme heterojunction efficiently promotes the spatial segregation of photogenerated charge carriers for participation in photoreactions. Herein, Ag₂S/Co_1-_xS@Co₉S₈@C (A-CCC) S-scheme heterojunction nanocatalysts was synthesized, demonstrating outstanding photocatalytic degradation efficiency under simulated solar light irradiation ranging from ultraviolet to near-infrared owing to strong interfacial electric field. Morphological and structural analyses via scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, Raman, and in-situ-X-ray photoelectron spectroscopy confirmed the retention of the Co-ZIF-67-derived octahedral morphology with uniform Ag₂S nanoparticle distribution and formation of distinct Co_1-_xS and Co₉S₈ phases embedded in a carbon matrix. Ultraviolet photoelectron spectroscopy and band gap measurements elucidated an S-scheme heterojunction configuration driven by an internal electric field, promoting interfacial charge. A steady-state THz time-domain spectroscopy in transmission mode and multi-exponential time resolved photoluminescence spectra fitting and calculated amplitude-weighted and intensity-weighted lifetimes (~2.38 ns) demonstrated significant interfacial charge separation within the 5A-CCC. The 5 wt% Ag₂S-CCC (5A-CCC) nanocatalysts endows exceptional photocatalytic activity for environmentally persistent antibiotic levofloxacin (LCN) degrading about 99.7% with an apparent rate constant of 0.0326 min^-1 in 40 min reaction duration due to extended light absorption till near infra-red region for effective solar to thermal conversion (13.6%). Radical scavenging and reactive oxygen species probe studies revealed O₂^•- as the dominant active species, participated effectively in LCN degradation. For LCN degradation, fragmentation and intermediate products were observed using liquid chromatography-mass spectrometer. This study features a highly effective photocatalytic system and offers essential insights towards full-spectrum functioning nanocatalysts for environmental detoxification of persistent antibiotics.

Key words: Persistent organic pollutants, Levofloxacin, Full-solar spectrum, S-scheme heterojunction, Interfacial charge transfer

Sangeeta Adhikari, Sandip Mandal, Do-Heyoung Kim. S-型Ag₂S/Co_1-_xS@Co₉S₈@C纳米催化剂用于多光谱太阳能驱动降解持久性有机污染物左氧氟沙星[J]. 催化学报, 2026, 89: 310-325.

Sangeeta Adhikari, Sandip Mandal, Do-Heyoung Kim. Multispectral solar-driven detoxification by S-scheme Ag₂S/Co_1-xS@Co₉S₈@C nanocatalyst of emerging persistent organic pollutant-levofloxacin[J]. Chinese Journal of Catalysis, 2026, 89: 310-325.

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图/表 10

Fig. 1. (a) Schematic synthesis process of the A-CCC nanocatalysts. HRSEM images of Co1-xS@Co9S8@C (b) and 5% Ag2S/Co1-xS@Co9S8@C (c,d) nanocatalysts.

Fig. 2. TEM, HR-TEM, and elemental mapping of Co1-xS@Co9S8@C (a-c) and 5 wt% Ag2S/Co1-xS@Co9S8@C (d-f). (g) XRD patterns of the synthesized nanocatalysts. Raman spectra (h) and FTIR spectra (i) of CCC, Ag2S, and 5A-CCC nanocatalysts.

Fig. 3. High-resolution XPS profiles of Co 2p (a), S 2p (b), and Ag 3d (c) in CCC, Ag2S, and 5A-CCC. (d) UV-vis spectra of the powdered nanocatalysts. (e) Tauc plots of Ag2S nanocatalysts. (f) PL spectra of the powdered nanocatalysts. (g) Photocurrent response of CCC, Ag2S, and 5A-CCC nanocatalyst electrodes with 10 s light on/o? intervals. (h) EIS spectra of CCC, Ag2S, and 5A-CCC nanocatalyst electrodes. (i) LSV spectra of CCC and 5A-CCC nanocatalyst electrodes.

Fig. 4. NIR thermal images of the CCC, Ag2S, and 5A-CCC nanocatalysts at different NIR illumination durations. CCC(a-e), Ag2S (f-j) and 5A-CCC (k-o). All images were captured by an infrared thermal imager

Fig. 5. (a,b) UPS spectra of CCC and Ag2S nanocatalyst. (c) Band structure configuration, IEF formation, and proposed S-scheme charge transfer mechanism at the 5A-CCC nanocatalyst heterojunction.

Fig. 6. Photocatalytic experiments under the irradiation of UV (a), Visible + NIR (b), NIR light (c), and full solar spectrum (simulated solar light) (d). (e) Degradation percentages under different light conditions. (f) Rate constants for CCC, Ag2S, and 5A-CCC nanocatalysts. (g) LCN degradation with varying 5A-CCC nanocatalysts amounts. (h) LCN degradation time vs. LCN concentration. (i) LCN degradation efficiency with effect of co-existing ions using 5A-CCC nanocatalysts under simulated solar light (error bars represent in Figs. 6(a)-(d) and 6(g)-(h), the standard deviation (SD ≤ ±2%) of three independent experiments under same conditions).

Table 1 Photodegradation efficiencies and kinetics for LCN over different nanocatalysts under simulated solar irradiation.

Catalyst	Adsorption (%)	Photooxidation efficiency (%)	k in 30 min (min^-1)	R²
LCN = 20 ppm, catalyst = 20 mg, and reaction time = 40 min
CCC	8	46.0	0.00377	0.99
Ag₂S	2	13.3	8.41E^-4	0.99
2A-CCC	15	66.0	0.0054	0.97
5A-CCC	17	99.7	0.0326	0.98
10A-CCC	16	73.0	0.0121	0.97

Fig. 7. (a) Cyclic photocatalytic LCN degradation by 5A-CCC nanocatalyst. Characterizations of spent 5A-CCC nanocatalyst after 7 consecutive cyclic experiments: (b) XRD pattern before and after catalysis action. High-resolution XPS of Co 2p (c), Ag 3d (d), and S 2p (e) from spent 5A-CCC nanocatalyst. (f) HRSEM micrograph of spent 5A-CCC nanocatalyst. (g) High-resolution TEM images of spent 5A-CCC nanocatalyst. (h) EDAX spectra obtained from HRTEM micrographs for spent 5A-CCC nanocatalyst after seven consecutives cycles.

Fig. 8. (a) Scavenger studies. (b) NBT concentration versus nanocatalyst. (c) PL spectra of 2HTA using CCC, Ag2S, and 5A-CCC nanocatalysts. (d) S-scheme charge transfer mechanism. (e) PRF comparison of the prepared nanocatalysts with reported catalysts from Table 2. (f) Radar plot includes catalyst concentration, pollutant concentration, degradation efficiency, reaction time, light source and PRF for nanocatalysts from Table 2 (A: CoWO4/Bi4O5I2; B: CaTiO3@Ag@ZnO; C: Bi2MoO6-SOVs/ZnCdS; D: Bi5O7I/Bi2O2CO3/Ag2CO3; E: B doped BiVO4/Bi; and F: 5A-CCC). (g) Schematic representation of Photocatalytic-Photothermal synergy in 5A-CCC nanocatalyst. (error bars represent in Fig. 8(a), the standard deviation (SD ≤ ±2%) of three independent experiments under same conditions).

Table 2 PRF values of different nanocatalysts used in photocatalytic LCN degradation in a wastewater system.

Catalyst	Cat. conc. (g L^-1)	Pollutant conc. (mg L^-1)	Degradation efficiency (%)	Reaction time (adsorption + photocatalysis in min)	Light source	PRF (mg W^-1 min^-1 L^-1)	Ref.
CoWO₄/Bi₄O₅I₂	0.5	5	86.3	40	300 W Xe-lamp	0.0071	[71]
CaTiO₃@Ag@ZnO	1	10	90	100	55 W Xe-lamp	0.0163	[72]
Bi₂MoO₆-SOVs/ZnCdS	0.625	20	95.9	30	300 W Xe-lamp	0.0106	[73]
Bi₅O₇I/Bi₂O₂CO₃/Ag₂CO₃	0.5	10	86.9	60	300 W Xe-lamp	0.0048	[74]
B doped BiVO₄/Bi	0.2	30	61.09	70	300 W Xe-lamp	0.00290	[75]
5A-CCC	1	20	99.7	40	150 W Xe-lamp	0.016	This work

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S-型Ag₂S/Co_1-_xS@Co₉S₈@C纳米催化剂用于多光谱太阳能驱动降解持久性有机污染物左氧氟沙星

Multispectral solar-driven detoxification by S-scheme Ag₂S/Co_1-xS@Co₉S₈@C nanocatalyst of emerging persistent organic pollutant-levofloxacin

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