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Surfaces and Interfaces · 2024 · IF 5.7

Advanced quasi-2D amorphous TiOx-Au photocatalyst: Harnessing defects and carriers transport to boost visible-light organic pollutants degradation

Jingting Su,Junyi Xia,Huijun Liang,Jun Xiao,Ruohu Zhang,Shuhong Xu,Li Zhu

Amorphous materials have recently garnered significant interest due to their low-cost fabrication methods, extensive surface area and plentiful surface defects , which offer numerous active sites for catalytic reactions . However, carriers self-trapping and recombination caused by bulk defects limit the employment of amorphous materials as photocatalysts . As such, it is essential to adjust the structure and defects to improve carriers utilization for creating high-performance amorphous photocatalysts. In this study, we developed a novel and facile strategy to fabricate a quasi-2D amorphous crepe-like TiO x -Au (cTiO x -Au) photocatalyst, in which the cTiO x was synthesized simply through one-step hydrolysis method at room temperature by constructing discrete reaction system with mass-confinement of the precursor to guide the morphology of the cTiO x . The removal efficiencies of the cTiO x -Au to antibiotic tetracycline (TC) and gaseous pollutant formaldehyde (HCHO) under visible light were 84.43 % and 95.92 %, respectively, which greatly surpassed those of its counterparts, normal amorphous TiO x (amTiO x )-Au (54.32 % and 73.67 %) and crystalline catalyst TiO 2 -P25-Au (49.29 % and 54.03 %). The remarkable visible-light photocatalytic capacity of cTiO x -Au can be attributed to the unique quasi-2D morphology of cTiO x . The ultrathin nanostructure not only maximizes surface defects and minimizes bulk defects, but also effectively shortens the carriers transport time and reduces recombination probability, on the other hand, it provides ample adsorption sites and accessible binding sites for plasmonic Au nanoparticles to amplify the effect of surface plasmon resonance enhancement. The excellent photocatalytic performances of cTiO x -Au for removing both aqueous and atmospheric pollutants endow it great potential in real environmental remediation applications.

研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Direct Z-scheme system of UiO-66 cubes wrapped with Zn0.5Cd0.5S nanoparticles for photocatalytic hydrogen generation synchronized with organic pollutant degradation

Dongfang Hou,Qian Zhu,Junjie Wang,Min Deng,Xiu-qing Qiao,Bojing Sun,Qingwen Han,Ruan Chi,Dong-Sheng Li

Optimized fabrication of Z-scheme photocatalyst based on MOF materials offers sustainable energy generation and environmental improvement due to their attractive properties. The Z-scheme heterojunctions consisting of UiO-66 cubes covered with Zn 0.5 Cd 0.5 S nanoparticles were fabricated by a facile solvothermal method. Thanks to the Z-scheme carrier transport under simulated sunlight irradiation, UiO-66@Zn 0.5 Cd 0.5 S exhibited enhanced photocatalytic performance of H 2 generation synchronized with organic pollutant degradation in fluoroquinolone antibiotic wastewater. Synergistically, the highest comprehensive performance was obtained in ciprofloxacin solution. The H 2 yield reached 224 μmol∙ g −1 ∙ h −1 and simultaneously the removal efficiency was up to 83.6 %. The degradation pathways revealed that the process of piperazine ring cleavage and decarboxylation also generates H protons, further promoting the production of H 2 . Therefore, the effective spatial separation and transfer of the photoinduced carriers are attributed to the good band structure, large specific surface area, and cooperative reduction and oxidation reactions of UiO-66@Zn 0.5 Cd 0.5 S, resulting in significant photocatalytic activity. The toxicity assessment of antibiotics and intermediate products during the photocatalytic reaction also verifies the reduction of environmental risk. This study highlights a promising way to expand the application of the MOFs-based photocatalyst in clean energy conversion coupling with water remediation.

研究领域: 材料科学 · 环境科学 · 能源科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

In-situ self-assembly of Z-scheme TiO2/g-C3N4 heterojunction enhanced visible-light photocatalytic performance for degrading phenolic pollutants

Ming Yi,Jiangwei Shang,Yunqing Liu,Xiuwen Cheng

In recent years, eliminating impurities from wastewater has become increasingly crucial. Photocatalytic technology has become a viable strategy for degrading organic pollutants. This study created novel Z-scheme TiO 2 -modified g-C 3 N 4 using a solvent-tunable, two-step method. The optimized TiO 2 /g-C 3 N 4 -Et/vis system demonstrated a removal efficiency of 94.4 % for acetaminophen (ATP) within 40 min and 91.0 % for methylparaben (MPB) within 100 min. Furthermore, the system maintained 92.7 % ATP degradation efficiency after five cycles, indicating excellent recoverability and sustainability. Photochemical tests and mechanistic studies revealed that solvent modulation and TiO 2 modification increased the specific surface area and facilitated the formation of Z-scheme heterojunctions. These heterojunctions effectively inhibit the recombination of photogenerated electron-hole pairs and enhanced the degradation efficiency of organic pollutants, primarily driven by •O 2 − . LC-MS analysis found the intermediates of ATP and MPB, and several potential routes of degradation were suggested. This work sheds fresh light on the production of high-performance TiO 2 /g-C 3 N 4 nanoparticles for applications related to energy and the environment.

CAS / MDL: 103-90-2 99-76-3
研究领域: 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

Cobalt-doped g-C3N4 as a heterogeneous catalyst for photo-assisted activation of peroxymonosulfate for the degradation of organic contaminants

Lingli Wang,Xu Guo,Yingying Chen,Shasha Ai,Hanming Ding

Cobalt-mediated peroxymonosulfate (PMS) activation is an effective way to generate sulfate radicals for the degradation of pollutants. Herein, a heterogeneous Co-based catalyst was prepared by integrating the cobalt species to the cavities of g -C 3 N 4 via the Co N bonds through the methods of impregnation and calcination, which was applied to activate PMS for the degradation of organic contaminates under visible light. The cobalt species were atomically dispersed on g -C 3 N 4 , which could provide more reactive sites for PMS activation. The catalytic efficiency of cobalt-doped g -C 3 N 4 was greater than that of pure g -C 3 N 4 or even slightly higher than that of the homogeneous cobalt ions during the photo-assisted PMS activation catalytic processes. The optimum Co loading is 1.0% in weight. In 25 min, the dye of rhodamine B was almost completely degraded with a 70.5% of total organic carbon (TOC) removal under its natural pH value in the presence of such catalytic system. The enhanced catalytic activity of Co-doped g -C 3 N 4 was due to the effective separation of the photo-generated charges as well as the sufficient accessible reactive sites for PMS activation. And the synergistic interaction between the photocatalytic and PMS activation processes facilitated the generation of active species for the removal of pollutants.

研究领域: 环境科学 · 催化化学 · 材料科学
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OPTICAL MATERIALS · 2022 · IF 3.754

TiO2@carbon microsphere core–shell micromotors for photocatalytic water remediation

Jian Lin,Yulian Tao,Jialiang Liu,Chan Zheng,Xiaoyi Song,Pingqiang Dai,Qianting Wang,Wei Li,Wenzhe Chen

Photocatalytic micromotors hold considerable promise for use in water remediation owing to the synergistic effect of a combination of photocatalytic activity and self-propulsive behavior. We designed a symmetric TiO 2 @carbon microsphere (CMS) core–shell micromotor with photocatalytic TiO 2 for enhanced degradation of organic contaminants. TiO 2 @CMS micromotors were obtained via a facile sol–gel method and subsequent heat treatment to obtain an anatase TiO 2 shell. The self-propulsion of TiO 2 @CMS micromotors is governed by asymmetric decomposition of H2O2 via asymmetric illumination of the spherical particles. The photocatalytic propulsion can be switched on and off by modulating the incident light. The speed of the photocatalytic TiO 2 @CMS core–shell micromotors can be increased by increasing either the light intensity or concentration of the chemical fuel, i.e., H 2 O 2 . In the degradation of rhodamine B, the photocatalytic performance of the micromotors was higher than those achieved with control group photocatalysts . The degradation efficiency reached ∼100% in approximately 60 min when all necessary conditions, i.e., use of micromotors, UV irradiation, and H 2 O, were applied. TiO 2 @CMS core–shell micromotors have the advantages of facile preparation, a simple structure, self-propulsion, and a high degradation efficiency and photocatalytic performance. They will therefore be important in the development of methods for water purification and wastewater treatment.

研究领域: 环境科学 · 材料科学
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WATER RESEARCH · 2019 · IF 7.913

Enhanced ronidazole degradation by UV-LED/chlorine compared with conventional low-pressure UV/chlorine at neutral and alkaline pH values

Xiang-Yun Zou,Yi-Li Lin,Bin Xu,Tian-Yang Zhang,Chen-Yan Hu,Tong-Cheng Cao,Wen-Hai Chu,Yang Pan,Nai-Yun Gao

Ultraviolet light-emitting diodes (UV-LEDs) are promising alternatives to conventional low-pressure UV (LPUV) lamps, mainly because they contain no toxic mercury and have a potential for less energy consumption and longer lifetime. In this study, UV sources including UV-LEDs (265, 275 and 285 nm) and LPUV (254 nm) were compared in UV/chlorine degradation of an organic contaminant , ronidazole (RNZ). UV-LED/chlorine performed better than LPUV/chlorine at neutral and alkaline pH values for RNZ degradation considering the fluence-based rate constant. However, the wall plug efficiencies of UV-LEDs are relatively low at present and must reach about 20–25% to achieve the same electrical energy per order as the LPUV in UV/chlorine degradation of RNZ at pH 7.5 and 9. Neither the contribution of radical (HO· or Cl·) nor the quantum yield of chlorine could explain the different RNZ degradation rate by UV/chlorine at different wavelengths and pH values, while the chlorine photolysis rate should be the key factor for these phenomena. The effects of common co-existing substances in real water (chloride, bicarbonate and natural organic matter) on UV/chlorine degradation of RNZ were similar at different UV wavelengths. Opposite to other oxidants or reductants, the molar absorption coefficient of chlorine increases when the UV wavelength increases from 254 to 285 nm at neutral and alkaline pH, which makes UV-LED/chlorine one of the best choices for UV-LED-based advanced oxidation/reduction processes.

研究领域: 环境科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

3D interconnected porous g-C3N4 hybridized with Fe2O3 quantum dots for enhanced photo-Fenton performance

Dong Liu,Chunling Li,Tianjun Ni,Ranpeng Gao,Jiayu Ge,Fengquan Zhang,Weidong Wu,Jinliang Li,Qian Zhao

Currently, the photo-Fenton oxidation has been increasingly studied in the domain of contaminant elimination. However, the lack of active sites and the slow charge migration in the catalytic process, still limit its practical application. 3D/0D hybrids offer a better opportunity for improving photo-Fenton activity due to their high charge mobility and increased number of catalytic sites, which is highly desirable but remains a large challenge. Herein, 3D interconnected porous g-C 3 N 4 hybridized with Fe 2 O 3 QDs (FCN) was developed and exhibited a porous structure and large specific areas. A large number of active sites and rapid charge separation/migration were achieved by the loading of ultrasmall Fe 2 O 3 QDs on the surface of g-C 3 N 4 . Moreover, the high charge mobility of this material promoted the fast conversion of Fe 3+ to Fe 2+ , resulting in the optimum synergistic effect between the photocatalytic and Fenton oxidation processes. Thus, the FCN catalysts exhibited excellent photo-Fenton oxidation activity towards the decomposition of organic contaminants (such as phenol, 2,4-dibromophenol, 2,4,6-trichlorophenol, rhodamine B and methyl orange). In addition, the roles of active species in the photo-Fenton oxidation reaction were also studied, and the results imply that the hydroxyl radicals played the most important role in the degradation of organic contaminants.

研究领域: 环境科学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 44 ·19013-19021 · IF 3.288

Efficient Z-scheme charge separation in WO3/PbWO4 for the removal of organic pollutants

Yi Zheng,Yiliang Shao,Xingzhi Jin,Min Shu,Longxiao Zhang,Chunlei Li

The contact quality of a composite is an important factor for the transfer and separation of photogenerated carriers. For this, we demonstrated a cation exchange method for the in situ construction of WO3/PbWO4 linked by WO6 octahedral crystal structure units, where WO3 was placed on the surface of PbWO4. We found that the apparent rate constant of the as-prepared WO3/PbWO4 was significantly increased (17 times higher than any single one). Our investigation indicated a remarkably enhanced photodegradation rate, originating from high contact quality. The photogenerated carriers of WO3/PbWO4 were greatly separated via the grain boundary, making WO3/PbWO4 exhibit 22 times higher photocurrent density than pristine PbWO4. Moreover, the photoelectrons and holes were separated through the high contact quality grain boundary built-in electric field, which is in accordance with the transmission path of the Z-scheme. Compared with the interface, a grain boundary is more conducive to the photocatalytic process. This study provides a feasible strategy to build a highly efficient Z-scheme photocatalyst with high contact quality grain boundary to remove organic pollutants.

CAS / MDL: 6080-56-4
研究领域: 材料科学 · 环境科学 · 光催化
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Molecular Catalysis · 2024 · IF 3.9

A Co-doped Ag3PO4 photocatalyst: Efficient degradation of organic pollutants and enhancement mechanism

Rui Lu,Jiaying Luo,Xuening Wang,An Chen,Yiwen Xie,Yang Xu,Tian Shang,Ruyan Li,Dongmei Jiang,Qingfeng Zhan

In this study, an efficient Co-doped Ag 3 PO 4 photocatalyst was prepared by the deposition method. Compared with Ag 3 PO 4 , the degradation efficiency of the optimal sample CAP-2 (the mole ratio of Co/Ag was 0.057 %) for MO (20 mgL −1 ) increased from 53.4 % to 95.0 % within 20 min, and the degradation efficiency for phenol (20 mgL −1 ) increased from 57.9 % to 91.8 % within 80 min. Moreover, the CAP-2 sample performed excellent mineralization ability and stable recycling capacity. Free radical capture experiments and electron spin resonance (ESR) measurements indicated that holes (h + ) and superoxide radicals (⋅O 2− ) were the main active radicals. Doping Co ions broadened the optical absorption, introduced impurity level to promote the separation of carriers, and generated additional ⋅O 2− owing to the mutual conversion of Co 3+ and Co 2+ , thus considerably improving Ag 3 PO 4 photocatalytic performance. This work provides a new reference for doping metal ions modified semiconductor photocatalysts to efficiently degrade organic pollutants.

CAS / MDL: 106-51-4 10026-22-9
研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Scalable synthesis of Ca-doped α-Fe2O3 with abundant oxygen vacancies for enhanced degradation of organic pollutants through peroxymonosulfate activation

Sheng Guo,Haojie Wang,Wei Yang,Hussain Fida,Liming You,Kun Zhou

In this work, a cost-effective and eco-friendly calcium-doped α-Fe 2 O 3 (Ca-Fe 2 O 3 ) with abundant oxygen vacancies was fabricated using a scalable precipitation-calcination method to activate peroxymonosulfate (PMS) for wastewater purification. Density functional theory calculations revealed that the incorporation of Ca 2+ into the α-Fe 2 O 3 structure enhances the electron transfer from α-Fe 2 O 3 to PMS, facilitating the activation of PMS. The degradation of Rhodamine B by 5%Ca-Fe 2 O 3 proceeded with a reaction constant 8 times higher than that of pristine α-Fe 2 O 3 . This can be attributed to the increased generation of 1 O 2 and O 2 • − , increased specific surface area and enhanced electrical conductivity. The applicability of the 5%Ca-Fe 2 O 3 /PMS system was investigated including its operating parameters and stability, and the intermediates involved in the reaction were identified. The 5%Ca-Fe 2 O 3 /PMS system exhibited excellent degradation efficiency in natural water samples. This work opens up new perspectives for designing highly efficient catalysts and renders iron oxides potential candidates for environmental remediation.

研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2019 · IF 5.108

Efficient degradation of refractory organic contaminants by zero-valent copper/hydroxylamine/peroxymonosulfate process

Huizhong Chi,Xu He,Jianqiao Zhang,Jun Ma

Degradation of naproxen, bisphenol S and ibuprofen in a hydroxylamine enhanced zero-valent copper (Cu 0 ) catalyzed peroxymonosulfate system was investigated for the first time. We found that hydroxylamine addition accelerated the reduction of Cu 2+ to Cu + as well as the corrosion of Cu 0 , and environmental friendly gas nitrogen was the main product of hydroxylamine. Additionally, hydroxyl radical and sulfate radical were identified to be the dominant reaction species by competitive experiments. The degradation of naproxen, bisphenol S and ibuprofen kept highly efficient in the pH range of 3.0–7.0 in Cu 0 /hydroxylamine/peroxymonosulfate process, with their degradation products identified by HPLC-MS, which showed that Cu 0 /hydroxylamine/peroxymonosulfate system could be an alternative to remove non-steroidal antiinflammatory drugs or plasticizers in wastewater. Furthermore, the effects of Cu 0 , hydroxylamine and peroxymonosulfate dosage were studied and optimized by a BBD based response surface model. This study provided a method to solve the disadvantages of Cu 0 /peroxymonosulfate systems, and gave a promising method to enhance the efficiencies of ZVMs activated system such as iron, cobalt and copper.

研究领域: 环境科学 · 化学工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Homogeneous catalytic activation of peroxymonosulfate and heterogeneous reductive regeneration of Co2+ by MoS2: The pivotal role of pH

Cong Pan,Libin Fu,Yaobin Ding,Xueqin Peng,Qihang Mao

The application of MoS 2 to enhance Co(II)/peroxymonosulfate (Co(II)/PMS) system for organic pollutants degradation was developed, and the mechanism for pH dependent catalytic activity in the MoS 2 co-catalyzed Co(II)/PMS processes was systematically investigated. It was found that MoS 2 presented enhancement effect for Co(II)/PMS system in the tested pH range from 4.0 to 7.0, especially at pH 5.5 and 6.0. The pseudo first order reaction rates for Rhodamine B (RhB) degradation in MoS 2 -Co 2+ /PMS system at pH 5.5 and 6.0 were 3.2 and 1.8 times that in Co 2+ /PMS system (Co 2+ 2 μmol L −1 , PMS 0.2 mmol L −1 , MoS 2 0.5 g L −1 ). The redox recycle of Co 3+ /Co 2+ was promoted by Mo(IV) and S(-II) on MoS 2 surface and regenerated Co 2+ induced homogeneous activation of PMS for the robust production of free radical with the major of hydroxyl radicals . Increasing MoS 2 dosage, Co 2+ and PMS concentration can linearly raise RhB degradation rate in MoS 2 -Co(II)/PMS system. Moreover, MoS 2 exhibited excellent catalytic and chemical stability in recyclability and reuse for catalytic decontamination in MoS 2 -Co(II)/PMS system. This work gains new insight into the enhancement effect of MoS 2 in the meal ions/PMS system, and provides a high performance wastewater treatment process of Co(II)/PMS at low concentrated Co 2+ .

CAS / MDL: 1317-33-5
研究领域: 环境科学 · 催化化学
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