Journal of Water Process Engineering
·
2025
·
IF 6.7
Zhou Shi,Chenxi He,Hao Huang,Xile Huang,Tong Hu,Yijia He,Dazhi Yang,Simeng Xia,Haojie Zhang,Lin Deng
The frequently detected antibiotics in aquatic environments can induce antibiotic-resistance genes, thereby posing significant risks to both ecosystems and human health. Thus, it is imperative to remove antibiotics from water environments. We constructed a novel polydopamine-loaded copper sulfide (CuS@PDA) through a simple hydrothermal method to activate H 2 O 2 to degrade tetracycline (TC). Compared to CuS/H 2 O 2 , the CuS@PDA/H 2 O 2 system not only achieved efficient TC removal with kinetic rate constant of 0.20 min −1 , but also showed much lower Cu 2+ ions leaching (3.81 mg/L from CuS vs. 0.21 mg/L from CuS@PDA). Besides, CuS@PDA exhibited remarkable recyclability with 93 % removal in the fifth consecutive cycle. Mechanisms analysis revealed that Cu and S contributed to the H 2 O 2 activation and S promoted the conversion of Cu(II) to Cu(I), beneficial for the production of reactive oxygen species. 1 O 2 was found to play the dominant role in the degradation of TC on the basis of quenching tests and electron paramagnetic resonance (EPR) analysis. PDA in CuS@PDA composites facilitated easier complexation with H 2 O 2 and conferred stronger oxidation capability. Lastly, the TC degradation pathway by CuS@PDA/H 2 O 2 was proposed, and the ecotoxicity of its degradation intermediates was estimated. In conclusion, this work demonstrates that the use of PDA can not only improve the catalytic activity and recyclability of CuS towards H 2 O 2 activation for organic pollutants degradation, but also greatly mitigate copper ions leaching.
研究领域:
环境科学
·
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ming Ma,Yuxin Lu,Sheng Wang,Shangkun Pei,Chong-Chen Wang,Xiang Li,Bo Wang
Slfamethoxazole (SMX) has been considered as one kind of important micropollutants in water which need to be removed effectively. Developing one kind of material for effectively removing SMX in water is crucial in treatment process. In this study, core–shell structured metal–organic frameworks (MOFs) with increasing shell thickness (5, 10, and 20-ZIF-8@ZIF--67 s) were selected as an ideal platform to develop water-stable hierarchical porous carbons (HPCs) using one-step calcination, showing the dual functionals of both adsorption and catalysis by producing large amount of acitve species ( 1 O 2 ). These novel HPCs systematically optimized at increasing temperatures and ratios of two metals. The 10-Co-NHPC-900 at optimal conditions shows highest adsorption capacities and initial adsorption rates, which are 4.56 and 10.35 times higher than those of calcinated ZIF-67 s. The decomposition mechanisms based on PMS were systematically studied by analyzing oxidant consumption, reactive oxygen species and by-products of SMX. In addition, Co ions leached amount of 10-Co-NHPC-900 was 63.6 times lower than that of MOF precursor, indicating that the cobalt-based porous carbon have higher water stabilities. This study offers an efficient approach for reducing micropollutants risk using water-stable hierarchical porous carbons.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Qian-Qian Tang,Bang-Xiang Wu,Xiao-Wen Huang,Yi Hu,Dongmei Hou,Wei Ren,Ling-Ling Liu,Ying Chen,Lei Tian,Long-Shuai Zhang,Qing Sun,Jian-Ping Zou
Highly selective generation of singlet oxygen ( 1 O 2 ) in the electro-Fenton system remains challenging due to susceptibility of the O-O bond to break in O 2 reduction reaction and activation process of H 2 O 2 . Herein, the nitrogen-coordinated Fe single-atom catalyst with a high coordination number (FeN 6 /CN) was synthesized, allowing the Fe sites to remain trivalent while presenting a high spin state. The quenching experiments and EPR tests proved that the electro-Fenton system of FeN 6 /CN achieved high selectivity generation of 1 O 2 , showing excellent degradation performance of different organic pollutants. Combined with theoretical calculations, the FeN 6 sites displayed a lower energy barrier for the transfer from *H 2 O 2 to 1 O 2 . In the FeN 6 /CN’s electro-Fenton system, the high spin state of FeN 6 site ensured generation of H 2 O 2 via 2e - reduction. Simultaneously, the high oxidation state of FeN 6 site further achieved a highly selective generation of 1 O 2 by in situ activation of H 2 O 2 in the electro-Fenton system. Particularly, the FeN 6 /CN’s electro-Fenton system showed a high energy-efficient for pollutant removal (23.79 kWh·kg toc −1 ) compared to other electro-Fenton systems (50–300 kWh·kg toc −1 ). The electronic structure regulation of single atom sites provides a new avenue for highly selective generation of 1 O 2 in the electro-Fenton system.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 2
·329
·
IF 3.9
Xueqing Ren,Peng Xu,Ke Tian,Menghan Cao,Fengyin Shi,Guangshan Zhang
The post-separation of powder catalysts restricts the practical application of peroxymonosulfate (PMS)-based advanced oxidation technology. Hence, we fabricated CuO-Fe2O3-modified Ni foam (CFO-NF) using a facile hydrothermal method for an efficient PMS activation. The CFO-NF/PMS system could achieve a 97.9% tetracycline hydrochloride (TC) removal efficiency in 60 min with four pieces of CFO-NF and 0.4 mmol L−1of PMS. The removal efficiency was maintained at ˃85% even after five cycles, indicating the excellent stability of CFO-NF composites. The conversion among Fe(III)/Fe(II), Cu(II)/Cu(I), and Ni(III)/Ni(II) accelerated the PMS decomposition, verifying the synergy between CuO-Fe2O3and Ni foam. The trapping experiments and EPR detection confirmed that abundant active species (•OH, SO4•−, O2•−, and1O2) were produced in the CFO-NF/PMS system, accounting for the existence of radical pathways and a non-radical pathway, in which1O2(non-radical pathway) was dominated. This study developed a novel CuO-Fe2O3-modified Ni foam with a superior PMS activation performance, a high stability, and a recoverability for eliminating refractory organic pollutants.Keywords:CuO-Fe2O3-modified Ni foam;peroxymonosulfate;tetracycline;stability;singlet oxygen
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Chao Qu,Yan-gang Li,Shu-juan Meng,Xiao-hu Li,Shu-jun Zhang,Da-wei Liang
Recently, carbon nanotubes coated carbon black and polytetrafluoroethylene (CNTs-C/PTFE) gas diffusion electrode was used as an air-cathode in an electro-oxidation (EO) system for effectively generating hydrogen peroxide (H 2 O 2 ) through a 2-electron oxygen reduction reaction (ORR). This ORR-EO system not only lowered applied voltage and conserved energy, but the synergistic peroxone (O 3 /H 2 O 2 ) reaction could increase hydroxyl radicals ( • OH) generation for organics elimination. However, a significant proportion of H 2 O 2 was left in the effluent of ORR-EO, which was a loss of resources and energy. In this study, a Fenton-like reaction for in-situ H 2 O 2 decomposition to generate active oxidation species was inserted by introducing MnO 2 into the cathodic catalyst layer, and the sole MnO 2 /CNTs-C/PTFE air-cathode could accomplish 90% of phenol degradation. When MnO 2 /CNTs-C/PTFE air-cathode combined with Ti/NATO anode in an ORR-EO system, all anodic oxidation, Fenton-like reaction, and peroxone took place to successfully generate • OH and singlet oxygen ( 1 O 2 ). Over 95% of TOC in phenol and landfill leachate bio-effluent was effectively eliminated, with 20% energy savings compared to the ORR-EO with CNTs-C/PTFE air cathode.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jiahao Zhu,Jianqing Ma,Sijing Yao,Mika Erik Tapio Sillanpää,Minghua Zhou,Chensi Shen,Qing Ye,Huixia Jin,Kefeng Zhang
Heterogeneous Fenton-like systems using H 2 O 2 as an oxidant have been extensively investigated in acidic and neutral conditions, but usually, they become ineffective under alkaline conditions. In this study, a cuprous graphitic carbon nitride material (Cu–CN) was prepared that can generate singlet oxygen ( 1 O 2 ) from H 2 O 2 . The results demonstrate that at pH 11, 95 % of 50 mg/L p -chlorophenol (4-CP) can be effectively eliminated within 120 min. Through semi-quantitative analysis and density functional theory calculations, it has been confirmed that 1 O 2 is the dominant reactive oxygen species in this system under alkaline conditions. The main pathway for 1 O 2 generation involves the formation of a complex between · O 2 – and Cu(II)-N sites, and the subsequent intramolecular electron transfer. To enhance the stability and separation performance of this catalyst, polyethylene glycol (PEG) was employed as a binder to combine Cu–CN with Fe 3 O 4 . The terminal hydroxyl groups in PEG were cross-liked by metals, thus forming a solid and magnetic composite (CuFe@PEG). Compared to Cu–CN, CuFe@PEG exhibited remarkable performance with 93 % retention of its original capacity for 4-CP removal at pH 11. Furthermore, after seven cycles, the degradation efficiency only decreased by 6.36 %. This study introduces a novel approach for utilizing Fenton-like reactions in treating alkaline wastewater.
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Lipeng Wu,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Herein, a series of Co@N–C materials are synthesized using nitrates (LiNO3, NaNO3, and KNO3) as templates to control the preferential growth of the cobalt (200) facet. Co@N–C–X (X = LiNO3, NaNO3, and KNO3) exhibit excellent activities and long-term stabilities for Fenton-like degradation of bisphenol A (BPA) with peroxymonosulfate (PMS) as an oxidant. The texture coefficient (TC) is used to investigate the relationship between the Co facets and their catalytic activities, and a linear relation is built between the TC of Co(200) and the reaction rate constant (k). Co(200) is therefore the most active facet for PMS activation, while nitrates can promote the preferential growth of the Co(200) facet. Moreover, the Co(200) facet is more stable against leaching and can achieve more quick transformation between Co2+/Co3+. Quenching tests, electron paramagnetic resonance spectra, and electrochemical tests show that singlet oxygen (1O2) plays the dominant role for BPA degradation. Density functional theory verifies that Co nanoparticles coated with a graphitic nitrogen-doped carbon layer have the best activity for PMS activation. This work first proposes the strategy of using nitrates to control the preferential growth of Co facets and reveals the relationship between the TC value and k, thus attracting great interest in the environmental field.
研究领域:
环境科学
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yandong Xu,Mengxia Guo,Chengjun Ge,Ping Zhang,Wen Xu,Linlin Zhang,Shihao Zhou,Jianjun Liao
To facilitate the activation of peroxymonosulfate, it is useful to simultaneously tune the coordination environment of the single-atom catalyst and develop a structure that effectively exposes the active site. In this study, we used a pre-assembly calcination method to prepare a structure composed of Cu single atoms on O-doped g-C 3 N 4 nanosheets (5Cu-OCN), and studied how this structure can effectively activate PMS under visible light catalysis. Compared to the g-C 3 N 4 , the 5Cu-OCN exhibits significantly improved PMS activation effect. Cu single atoms play an important role in catalyzing PMS activation and removing carbamazepine from solution, and explain the contribution of photo generated electrons and holes in enhancing the performance of catalysts in PMS activation. Furthermore, the constructive cooperation of 5Cu-OCN photocatalysts by PMS activation and photocatalysis has been shown to be useful in real aqueous systems. The results indicate that the main pathway for the generation of 1 O 2 is through the 5Cu-OCN photocatalytic process to promote PMS activation. In addition, the active reaction species involved in the degradation of carbamazepine were identified. This study provides an efficient copper monoatomic catalyst that can react to visible light for 1 O 2 based advanced oxidation processes.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124526
·
IF 7.5
You Zhou,Zhiquan Yang,Siyuan Di,Huarong Yu,Fangshu Qu
Addressing antibiotic water pollution through novel and effective strategies has become a critical endeavor. Increasing studies have shown that peroxymonosulfate (PMS) can be activated to generate singlet oxygen ( 1 O 2 ) by incorporating transition metals into carbon-based materials. Hollow carbon nanocages (HCNs) have proven to be a promising material for advancing energy conversion and battery technologies. However, studies based on HCNs in the field of Fenton-like reactions are scarce. In this study, the Fenton-like activity of HCNs-based catalysts were enhanced via confinement effect coupled with asymmetric Si coordination configuration. The hollow architecture endowed the catalyst with accelerated mass transport and markedly elevated utilization efficiency of active species. Co-HCNs delivered exceptional catalytic performance, accomplishing 99% tetracycline (TC) degradation within 40 min with a 67% mineralization rate, combined with robust anti-interference capacity in real-world water matrices. Density Functional theory (DFT) calculations indicated that the carbon-dense layer boosts the generation of 1 O 2 , in contrast to the cobalt core, which predominantly induced radical-mediated pathways. Integrated experimental analyses further confirmed that the degradation process is dominated by 1 O 2 , with other radicals playing synergistic contributions. Ecotoxicity evaluation verified the environmental compatibility of this process. This work further reveals an "oxidant-derived, dual-channel-driven 1 O 2 supply mechanism." This mechanism enhances the instantaneous supply capacity of 1 O 2 in the system and provides a clearer catalytic rationale for the selective oxidation of pollutants and stable purification in complex water matrices.
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2026
·
IF 12.8
Xuan Qu,Qian Xu,Zhiqiang Chen,Ang Li
Reactive oxygen species (ROS) generated on or near the oil droplet surface have remarkable potential in altering the structure of 1-adamantanecaboxylic acid (ACA) at the oil-water interface, facilitating separation of oil and water. To stimulate confined multi-phase ROS, a thermodynamic control strategy for ozone catalysis by Fe clusters anchored on nanoscale supports was developed. This strategy explored interfacial pollutant redistribution within film of microdroplets (10-20 μm in size) prepared with a high-speed shear emulsifier. Experimental results indicated that 1 O 2 selectively attacked carboxylic groups confined at the oil-water interface and two-electron migration pathway from ACA to adsorbed O 3 at interfacial oxygen vacancies (O v ) led to spatial redistribution with hydrophilic dihydroxylated intermediates via synchronous electrophilic substitution. ACA attached to interface of microdroplet is fueled by •OH and 1 O 2 , achieving degradation at 89.84% within 30 min, and pseudo-first-order kinetics rate constants ( k obs ) of 0.0793 min –1 . Thermodynamic analysis revealed that 1 O 2 reduced the Gibbs free energy (Δ G ) by 23.98 kJ mol −1 relative to that of •OH. This phenomenon is attributed to the narrow site distribution of Fe clusters, which enhances the overall electron utilization efficiency. These findings demonstrate the feasibility of manipulating ROS to regulate the distribution of interfacial species, representing a promising strategy for promoting the coalescence of oil microdroplets.
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wei Sun,Mushan Xie,Bo Shi,Zhixuan Zhu,Jian Zhang,Ying Wang,Jing Bian,Haibo Wang,Chun Zhao
The selective and simultaneous removal of antibiotics (ABs), antibiotic-resistant bacteria (ARBs), and antibiotic resistance genes (ARGs) from complex water matrices is crucial but remains challenging. Herein, relatively pure nonradical oxidation systems of singlet oxygen ( 1 O 2 ) and reactive trivalent manganese (Mn( III ) aq ) were established through electrofiltration-activated peroxymonosulfate and permanganate processes, respectively. Both systems simultaneously removed ABs, ARBs, and > 99 % of 20 selected ARGs within 15 min, while the addition of anions and nature organic matter slightly inhibited ARB inactivation. A multiperspective investigation confirmed that 1 O 2 demonstrated superior efficacy in ARB inactivation and protein damage compared to Mn( III ) aq , whereas Mn( III ) aq destroyed the ARB cell membrane, induced oxidative stress, and damaged almost all ARGs more rapidly than 1 O 2 . In particular, 1 O 2 exhibited selectivity toward four ARGs, which was attributed to a positive dependence on the 5′-GG-3′ doublet content. Moreover, 1 O 2 and Mn( III ) aq significantly reduced the risks of ARB regrowth and horizontal gene transfer of ARGs while providing resilience in real water matrices with improved energy-effectiveness. The findings of this study offer new insights into nonradical reactive species dominated advanced oxidation processes for controlling antibiotic resistance in real water.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Wenhao Li,Xiunan Cai,Xintao Zhou,Zhongqiu Luo,Cuirong Yan,Jiayi Ge,Zuqiang Huang,Yanjuan Zhang,Pingyan Wang,Yongming Luo,Jiguang Deng
Remediation of antibiotic-contaminated water demands advanced oxidation processes with efficient singlet oxygen ( 1 O 2 ) generation. Conventional catalysts, however, suffer from limited active sites and sluggish radical production. Herein, a self-assembly tethering strategy is innovatively developed to precisely and simultaneously regulate the hollow tubular morphology and atomic coordination structure of cobalt single atoms anchored on boron-doped carbon nitride (CN). This yields a Co-N 3 B 1 catalyst for peroxymonosulfate (PMS) activation. Morphological reconstruction from bulk to hollow tubular CN exposes abundant active sites for PMS adsorption, while coordination engineering tailors the Co-N 3 B 1 configuration. Boron doping induces electron redistribution via p-d orbital hybridization, creating dual adsorption sites and optimizing PMS activation. The optimized Co-N 3 B 1 exhibited excellent catalytic performance for tetracycline hydrochloride degradation with a rate constant of 1.337 min −1 and a high 1 O 2 selective generation of 98.55 %. Combined experimental and theoretical studies reveal that the tailored Co electronic structure lowers the adsorption energy of PMS, enhances electrons donation of PMS, and reduces the energy barrier for 1 O 2 formation from *O intermediates (2.3–2.09 eV), facilitating O−O bond cleavage. Additionally, the doped B 2p orbitals effectively accept Co 3d electrons, thus weakening the Co−O bond between Co and PMS, enabling highly selective generation of 1 O 2 . This work provides a universal strategy for rational and precise modulation of specific reactive species in environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）