CHEMOSPHERE
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2019
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IF 5.108
Jiajun Long,Longqian Xu,Linghui Zhao,Huaqiang Chu,Yunfeng Mao,Deli Wu
In this study, Cu(0) was synthesized with NaBH 4 as a reducing agent for Cu(II) and used to activate dissolved molecular oxygen (O 2 ) under acidic conditions. The Cu(0) synthesized had much higher activity than the purchased. The roles of Cu was clarified and the formation of reactive oxygen species was discussed through direct detection for the first time. By detecting the valence change of Cu in a CuO system, Bisphenol A (BPA) was found to accelerate the transformation of Cu(II) to Cu(I). Besides, the evidence from electron spin resonance (ESR) studies and scavenging tests revealed the new roles of Cu(0) that Cu(0) could not only convert O 2 to produce ·O 2 − , but also catalyze H 2 O 2 to ·OH. The results from this study offer evidence of new reaction pathways in Cu-activated O 2 systems and deepen understanding of the reaction between Cu species and O 2 .
研究领域:
环境科学
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化学
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材料科学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 34
·17657-17669
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IF 11.301
Xiaoli Li,Ting Wang,Xueqin Tao,Ganhua Qiu,Can Li,Benxia Li
Metal-modified semiconductors are being deemed as one of the most promising photocatalysts for various applications. Although great efforts have been devoted to developing a variety of metal-modified semiconductor photocatalysts, the exact functions of their interfaces in governing photocatalytic processes still remain elusive. Herein, the interfacial synergy of metal sites and defective semiconductor with oxygen vacancies (VOs) was investigated toward the photocatalytic selective oxidation of toluene, by taking the Pd/BiOBr photocatalyst as an example. The presence of Pd induces the generation of more VOs on the BiOBr surface due to the electronic interaction at the Pd–BiOBr interface. The coexistence of the Pd and VO sites on BiOBr enables the favorable adsorption of O2 and toluene molecules. The Pd–BiOBr interface governs the charge separation and prompts the activation of O2 and toluene, leading to 1.5 times the activity of BiOBr–VO for the photocatalytic selective oxidation of toluene to benzaldehyde with a high selectivity (>99%). Moreover, the typical influencing factors, such as the illumination intensity and toluene concentration, were optimized to improve the photocatalytic efficiency. The active species and intermediates in the photocatalytic reaction were identified by a series of controlled experiments, as well as in situ ESR measurements. Therefore, both experimental and theoretical results provide the direct evidence to understand the key roles of the interfacial Pd and VO sites in enhancing photocatalysis toward the selective oxidation of toluene.
研究领域:
材料科学
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环境科学
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催化
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化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Fangfang Duo,Mingliang Zhang,Xiaoting Feng,Chubei Wang,Liangliang Chu,Xi Chen,Jianwei Zhou
Constructing Z-scheme heterojunction has been regarded as a fascinating method to enhance the charge carrier separation rate and retain the high photoredox ability. In this paper, a novel 0D/2D MoS 2 QDs/BiOCl Z-scheme heterojunction with outstanding visible-light photocatalytic performance has been successfully prepared by a facile one-step strategy. The MoS 2 QDs with a diameter of 5 nm were uniformly distributed on the surface of BiOCl nanosheets . The optimized MoS 2 QDs/BiOCl heterojunction showed the most robust CIP and RhB degradation efficiency, which was approximately 32.2 and 44.7 times higher than that of pure BiOCl under visible light irradiation, respectively. This result can be attributed to the synergetic effects of up-conversion and direct Z-scheme heterojunction of the MoS 2 QDs. The optical property , morphology and surface feature of the catalyst were analyzed through the UV–vis DRS, PL , XRD , Raman, FT-IR, XPS, SEM and TEM. The study of ESR characterization and free radical capture experiments confirmed the Z-scheme heterojunction electron transfer route. Finally, a rational photocatalytic mechanism for pollutants degradation over the MoS 2 QDs/BiOCl heterojunctions were proposed. This study may provide a reliable strategy for the construction of Z-scheme bismuth-based heterojunction and its potential application in photocatalytic organic pollutants degradation.
研究领域:
材料科学
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光催化
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环境科学
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纳米技术
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产品关联
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Ahsan Nazir,Ameena Tur Rasool,Chuntao Chen,Bianjing Sun,Dongping Sun
In this study, a NiO-PbBiO 2 Br photocatalyst was developed by a simple chemical precipitation approach followed by a hydrothermal process to eliminate tetracycline (TC). The resultant materials were assessed utilizing diverse characterization techniques. Compared with pure PbBiO 2 Br (49.5 %) and NiO (56.8 %), the NiO-PbBiO 2 Br composite exhibited superior photocatalytic effectiveness for removing TC under visible light and achieved a remarkable 98.4 % elimination of TC within 70 min (conditions: [TC] = 10 mg/L, pH 7 and [catalyst] = 1 g/L). The reaction rate constant (K) values are in the following order: NiO-PbBiO 2 Br (0.0591 min −1 ) > NiO (0.0119 min −1 ) > PbBiO 2 Br (0.0097 min −1 ). The markedly improved photocatalytic efficiency of NiO-PbBiO 2 Br can be ascribed to the expanded light absorption and the establishment of p-n heterojunction amid NiO and PbBiO 2 Br. The effects of several important factors, e.g. TC concentration, pH, catalyst dosage, and different water sources, were thoroughly investigated. Cycle tests were performed to confirm the stability and reusability of NiO-PbBiO 2 Br. Furthermore, electron spin resonance (ESR) and radical scavenging studies verified that the species •O 2 − , h + , and •OH play a key role in removing TC. The susceptible active regions of TC and the probable TC degradation routes were examined through density functional theory (DFT) calculations and high-performance liquid chromatography (HPLC) analyses. Thus, this work presents a new methodology for creating a photocatalyst with enhanced photocatalytic effectiveness for removing organic pollutants in water.
研究领域:
环境科学
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材料科学
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化学
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水处理
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计算化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Gaozu Liao,Peng Xu,Ping Lu,Xiaojiao Qing,Zhanjiang Yu,Yu Chang,Weirui Chen,Yiming Tang,Jing Wang,Xi Wang,Xukai Li,Laisheng Li,Dehua Xia
Single Co atoms dispersed on CMK-3 was synthesized and employed as efficient catalyst to degrade APAP in O 3 /PMS process. The results of morphology and structure characterization indicated that the as prepared catalyst possessed uniform array of mesoporous channel structure with a long-range. Co atoms were single atomic dispersed in CMK-3 skeleton with the form of CoN 4 coordination. The BET surface area and average pore diameter of 3.6% SA Co/CMK-3 were measured as 956 m 2 /g and 3.6 nm, respectively. For APAP degradation by 3.6% SA Co/CMK-3 + PMS/O 3 process, TOC removal efficiency reached to 60% and 78.9% in initial 1 min and 15 min, respectively. The influence of initial pH was investigated and demonstrated that APAP could be efficiently mineralized in a wide pH range. In addition, high mineralization rates were also achieved for other refractory organics (nitrobenzene and sulfamethoxazole). Radical quenching experiments and ESR indicated that SO 4 •− , •OH and 1 O 2 were all responsible for APAP degradation. DFT simulations elucidated that single Co atoms and N-heteroatoms on 3.6% SA Co/CMK-3 served as dual reaction sites for PMS and O 3 decomposition, which enhanced the ROS generation and APAP mineralization.
研究领域:
环境科学
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催化
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水处理
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DOI
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 20
·8015-8027
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IF 4.569
Zongyu Zhang,Xiuling Xue,Xiaoyi Chen
A novel ternary dual Z-scheme 2D g-C3N4 nanosheet/Ag3PO4/α-Bi2O3 (CNN/AP/BO) photocatalyst was successfully synthesized by an in situ deposition and hydrothermal–calcination method. The coupling of AP and BO remarkably enhanced the photocatalytic tetracycline (TC) degradation under visible light illumination, with an optimal removal efficiency of 91.6% (60 min), which can be attributed to the extended visible-light absorption and increased specific surface area owing to the interfacial intimate coupling with well-matched energy band positions between semiconductors. The improved photocatalytic activity resulted from the abundant free radicals by the order of ˙O2− > h+ > ˙OH based on the electron spin resonance (ESR) and quenching experiment results. In addition, the possible mechanism of TC degradation over the ternary dual Z-scheme heterojunction CNN/AP/BO was proposed.
研究领域:
材料科学
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环境科学
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光催化
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Qianqian Chen,Xiaobing Yang,Xingping Fu,Junjie Pan,Junmei Zhou,Gengwu Zhou,Kejun Cheng
Currently, antibiotics are extensively utilized in the pharmaceutical industry to assist humans and animals in combating various infectious diseases. The extensive use of various antibiotics enhances the quality of life. However, it can also have negative effects on the environment and human health, including water pollution and the rise of antibiotic-resistant microorganisms. To date, antibiotics have been detected in rivers, groundwater, and even drinking water. There is an urgent need to design and develop advanced materials for the remediation of antibiotics present in our environment. In this paper, we successfully synthesized a novel Ag 2 S-ZnS/ZIF-8 hollow heterojunction via facile sulphuration and solvothermal methods. This heterojunction was employed as a catalyst for the degradation of tetracycline (TC) in water under UV and visible light irradiation. The physicochemical properties of the as-synthesized catalysts were thoroughly analyzed using XRD, EDS, SEM, BET, XPS, TEM, ESR, UV–vis techniques. The results demonstrate that Ag 2 S-ZnS/ZIF-8 displays enhanced photocatalytic activity for TC degradation no matter under visible or UV light irradiation. After 10 min of UV light irradiation, its photocatalytic degradation efficiency was achieved 92.74 %. Additionally, Ag 2 S-ZnS/ZIF-8 was able to degrade 92.14 % of TC (visible light, with 35 min). The corresponding kinetic rate constant of Ag 2 S-ZnS/ZIF-8 is 0.145 min −1 (UV light) and 0.043 min −1 (visible light), respectively. Furthermore, Ag 2 S-ZnS/ZIF-8 also shown excellent stability for the degradation of TC in the presence of visible light. This is a result of its high specific surface area, superior photocurrent and efficient separation of photo-generated electrons-hole pairs. Apart from this, the photocatalytic degradation mechanism of TC over Ag 2 S-ZnS/ZIF-8 is discussed in detail.
研究领域:
环境科学
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材料科学
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化学
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纳米技术
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
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IF 6.182
Huiyong Li,Zemin Zheng,Mofan Liu,Hao Jiang,Dafeng Hu,Xudong Zhang,Lei Xia,Xuemin Geng,Jiangwei Lu,Xinran Cheng,Yanfen Wan,Peng Yang
A novel Pd nano-skeleton (Pd NSs) modified Bi 2 MoO 6 balls photocatalyst was prepared by a facile hydrothermal treatment. The characterization by multiple techniques demonstrated the excellent light absorption and effective photo-generated electron-hole pairs separation performance of the composite catalyst, which further proved its superior photocatalytic property. Compared to the pure Bi 2 MoO 6 nanosheets, carbon quantum dots (CQDs) modified Bi 2 MoO 6 balls and Pd nanoparticles (Pd NPs) modified Bi 2 MoO 6 balls catalysts, 1.3% Pd NSs@Bi 2 MoO 6 sample exhibited the optimal catalytic performance for removing methyl orange (MO), methylene blue (MB), K 2 Cr 2 O 7 , phenol and the simulated wastewater mixture formed by the first three above under the illumination of visible light. Above all, the degradation efficiency increased about 5 times that of the pure Bi 2 MoO 6 balls for the degradation of MO. This great improvement was mainly attributed to Pd NSs with many contact edges, which provided more active sites for the adsorption reaction of organic dye molecules, following its better near-infrared light absorption capacity in the catalytic system. The active species mainly involved in the reaction were verified by ESR technique and the trapping test, mainly involving O 2 − , holes, OH, etc., and a possible photocatalytic reaction mechanism and pollutant degradation pathway were also proposed.
研究领域:
环境科学
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化学
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材料科学
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水处理
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DOI
高影响因子
OPTICAL MATERIALS
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2021
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IF 3.08
Kun Jiang,Jin Zhang,Yingfei Wan,Zengjian Liu,Jinwei Chen
In order to obtain the advanced photocatalyst with high performance for removing the gaseous formaldehyde, a new strategy with amination of titanium dioxide (TiO 2 ) and combination with reduced graphene oxide (rGO) is proposed in this work. TiO 2 was first aminated into amino-TiO 2 and then combined with rGO by an electrostatic self-assembly process to form the amino-TiO 2 /rGO photocatalysts. The structure and morphology were characterized by XRD , FTIR, and SEM, respectively. Physicochemical properties were measured by EIS, XPS , ESR , PL , and photocurrent measurements. The mechanism of the photocatalytic reaction was studied. Optimal amino-TiO 2 /rGO catalyst exhibits high catalytic activity and recyclability. The reaction rate constant of HCHO over this catalyst is approximately 9.8 × 10 −3 L mol −1 ·min −1 , which is 10.5 times higher than that of the commercial Degussa P25 TiO 2 . The analysis results from XPS and ESR indicates that the high catalytic activity could be mainly attributed to the imine formed by chemisorption of amino and HCHO. The reaction speed of formaldehyde photolysis increases as the concentration of HCHO on the photocatalyst surface increased. In addition, the introduction of graphene enhances carrier separation efficiency so that leads to more reactive radicals such as hydroxyl radicals (·OH) and superoxide radicals (·O 2 − ), leading to improved performance on formaldehyde photolysis. This could provide a useful method for highly efficient formaldehyde photocatalysis .
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
研究领域:
环境科学
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化学工程
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等离子体化学
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污水处理
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Zihao Cui,Qianqian Zhang,Hui Fu,Qihao Liu,Xiaolei Liu,Yaqiang Wu,Peng Gao,Zeyan Wang,Zhaoke Zheng,Hefeng Cheng,Yuanyuan Liu,Ying Dai,Baibiao Huang,Peng Wang
Herein, a facile anti-solvent preparation strategy is proposed to fabricate lead-free halide perovskite Cs 3 Bi 2 Br 9 with TiO 2 , which boosts photocatalytic activation of C(sp 3 )−H bonds in toluene oxidation . TiO 2 not only works as nucleation center to reduce the particle size of perovskite, but could form type II heterojunction with Cs 3 Bi 2 Br 9 , thus improving the photocatalytic performance of the TiO 2 /Cs 3 Bi 2 Br 9 composite. Under AM 1.5 G simulated sunlight irradiation, the optimal TiO 2 /Cs 3 Bi 2 Br 9 composite exhibits both high production rate (9692.5 μmol g −1 h −1 ) and selectivity (91 %) of benzaldehyde product. As verified by in-situ ESR, in-situ FT-IR and DFT calculations, •O 2 − and h + are demonstrated to be the main active species in this process. This work provides a new insight into the design of high-performance lead-free perovskite photocatalysts for organic synthesis.
研究领域:
材料科学
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光催化
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有机合成
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纳米技术
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产品关联
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·2982-2994
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IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）