JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Boqiang Li,Baiyang Chen,Zongsu Wei
UV/peroxydisulfate (UV/PDS) process is known to be highly efficient for degrading micropollutants from water by generating sulfate (SO 4 •− ) and hydroxyl radicals (HO • ). Reliable analyses of short-lived SO 4 •− and HO • are therefore critical for understanding reaction mechanisms and optimizing operating conditions. Currently, alcohols are commonly used as quenchers to distinguish radicals based on the assumption that they exclusively react with target radicals without other influences. However, this study for the first time reveals a series of unexpected effects that challenge this conventional wisdom because: 1) adding alcohols altered the decomposition rates of PDS by replacing the reactions between SO 4 •− and HO • with PDS by the reactions between secondary reactive species and PDS; and 2) SO 4 •− preferably reacted with alcohols to generate nonnegligible level of hydrogen peroxide (H 2 O 2 ) under oxygen-rich conditions, which subsequently led to indirect formation of HO • . Additionally, the formation of H 2 O 2 was substantially impacted by the types of alcohols, dosages, dissolved oxygen, and solution pH. Using probe tests as tools, we found that the actual SO 4 •− levels after dosing alcohols were only slightly different from assumed/expected levels, whereas the actually HO • levels were 43.7, 3364.9, and 12.5 times higher than assumed/expected conditions for samples dosed with methanol, iso-propanol, and tert-butanol, respectively. These unanticipated effects thus suggest that cautions are needed when using alcohols to qualitative and quantitative determine HO • and SO 4 •− in UV/PDS process.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Xin Huang,Man Su,Jizhi Zhou,Weikang Shu,Zhifeng Huang,Naiyun Gao,Guangren Qian
Persulfate based advanced oxidation processes have been well investigated, with the generation of radical species via various activation methods. This study reports an activation pathway of peroxydisulfate (S 2 O 8 2− , PDS) without radical production, achieved by the intercalation of PDS into Mg/Al-layered double hydroxide (LDH). Physical characterization indicated that the LDH was intercalated by PDS with the interlayer distance increasing to 0.917 nm. Approximately 93.9% of the phenol was decomposed by a LDH-PDS composite containing 0.4 mmol/g PDS, whilst no removal of phenol was achieved in the control group with PDS. Moreover, sulfate from decay of PDS was likely kept in the layers of LDH for no sulfate leakage in solution was observed. This is in accordance with the occurrence of characteristic peaks assigned for sulfate in FT-IR spectrum of LDH-PDS after reaction. Interestingly, radicals were not recorded by electron spin resonance measurement or radical scavenger tests during the oxidation process. The reactivity of PDS was likely improved by the basic sites on the LDH laminate, which provided OH to activate the O O bond in PDS. Further, the limited space of LDH layers reduce the bond cleavage of intercalated PDS and thus the generation of radicals. Therefore, the results proposed a non-radical reaction between phenol and PDS in the interlayer of LDH and developed a novel activation pathway for PDS in the elimination of organic contaminants.
研究领域:
环境科学
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化学工程
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高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Binshu Sun,Jianhong Zheng,Dewu Yin,Huile Jin,Xin Wang,Quanlong Xu,Aili Liu,Shun Wang
Cocatalyst can greatly facilitate the charge separation efficiency and decrease the activation barrier of a specific reaction, thus contributing the improved photocatalytic performance. Herein, PdS/CdS/MoS 2 was synthesized via a facile microwave-assisted approach. Owing to the coexistence of PdS and MoS 2 , respectively serving as oxidation and reduction cocatalyst, PdS/CdS/MoS 2 displayed enhanced photocatalytic performance in both hydrogen production (6610 μmol·g −1 ·h −1 ) and benzylamine oxidation (87% conversion) in comparison with the individual and binary composite counterparts. The improved photocatalytic activity was mainly attributed to the high charge separation efficiency and lowed activation barrier. Furthermore, the introduction of PdS can timely extract photogenerated holes from CdS, which effectively inhibits the photo-corrosion of CdS, endowing it with high stability. This work paves the way for developing efficient chalcogenide photocatalysts.
研究领域:
材料科学
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光催化技术
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DOI
高影响因子
ACS ES&T Engineering
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2022
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IF 0
Shaoxiong He,Enya Wu,Mingjie Shen,Haodong Ji,Lixi Zeng,Mingshan Zhu
Fluorinated liquid crystal monomers (LCMs) have been identified as emerging persistent and bioaccumulative chemicals with non-negligible environmental concentrations. Herein, 12 fluorinated LCMs including highly detected 4-ethoxy-2,3-difluoro-4′-(trans-4-propylcyclohexyl)biphenyl (EDPB) were selected as target fluorinated LCMs to investigate their structure–reactivity relationships by the ultraviolet/peroxydisulfate (UV/PDS) treatment. EDPB with biphenyl and ethoxy showed the highest first-order degradation rate constant of 1.93 h–1, while that of fluorinated LCMs with ethoxy (1.10–1.26 h–1) and biphenyl (0.45–0.56 h–1) and without biphenyl or ethoxy (0.27–0.30 h–1) decreased sequentially. HO• and SO4•– were identified as the main oxidative species in the UV/PDS treatment. Theoretical calculation suggested that biphenyl and ethoxy can significantly alter the electron distribution of LCM molecules, providing more attackable sites for HO• and SO4•– on LCMs with biphenyl or ethoxy. Oxalic acid, cyclohexane, and bicyclohexane were the main degradation products of fluorinated LCMs even though their degradation pathways were determined by their different molecular structures. Toxicity estimation revealed that fluorinated LCMs with high acute toxicity and developmental toxicity could be decomposed into some final products with less toxicity. This study is expected to fill knowledge gaps in the structure–activity relationships of fluorinated LCMs by the UV/PDS treatment.
研究领域:
环境科学
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化学工程
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Bo Feng,Kaining Sun,Guangbo Che,Tianyi Yang,Yongya Zhang,Qianqian He,Tianrui Chang,Lijing Wang,Renquan Guan
To address the need for efficient catalysts that excel in persulfate (PDS) activation and carrier extraction, a gadolinium oxide (Gd 2 O 3 ) modified strontium titanate (SrTiO 3 ) photocatalyst has been devised for the photo-Fenton reaction, targeting the degradation of tetracycline and ciprofloxacin. This innovative photocatalyst harnesses the formation of a heterojunction between Gd 2 O 3 and SrTiO 3 , which dramatically enhances PDS activation and boosts carrier extraction efficiency by 6.8 times. Notably, it achieves approximately 90% degradation of tetracycline across various pH levels and approximately 80% degradation of ciprofloxacin under acidic and neutral conditions. Importantly, the photocatalytic treatment significantly mitigates the biotoxicity of the degraded antibiotics, emphasizing its environmental safety and efficacy. The underlying mechanisms of PDS activation and carrier transport have been rigorously verified through theoretical calculations, while the potential photocatalytic pathways and mechanisms of antibiotic degradation have been elucidated using Fukui function analysis and liquid chromatography-mass spectrometry (LC-MS). This comprehensive approach underscores the photocatalyst’s potential for advanced environmental remediation applications.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Sui-Qin Yang,Rui-Qiu Ye,Yu-Hong Cui,Zheng-Qian Liu,Kai Sun,Yu-Ze Yu
Advanced oxidation processes for the treatment of organic pollutants in wastewater suffer from difficulties in mineralization, potential risks of dissolved residues, and high oxidant consumption. In this study, radical-initiated polymerization is dominated in an UV/peroxydisulfate (PDS) process to eliminate organic pollutant of pharmaceutical metoprolol (MTP). Compared with an ideal degradation-based UV/PDS process, the present process can save four fifths of PDS consumption at the same dissolved organic carbon removal of 47.3%. Simultaneously, organic carbon can be recovered from aqueous solution by separating solid polymers at a ratio of 50% of the initial chemical oxygen demand. The chemical structure of products was analyzed to infer the transformation pathways of MTP. Unlike previous studies on simple organic pollutants that the polymerization can occur independently, the polymerization of MTP is dependent on the partial degradation of MTP, and the main monomer in polymerization is a dominant degradation product (4-(2-methoxyethyl)-phenol, denoted as DP151). The separated solid polymers are formed by repeated oxidation and coupling of DP151 or its derivatives through a series of intermediate oligomers . This proof-of-concept study demonstrates the advantage of polymerization-dominated mechanism on dealing with large organic molecules with complex structures, as well as the potential of UV/PDS process for simultaneous organic pollution reduction and organic carbon recovery from aqueous solution.
研究领域:
环境科学
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水处理工程
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药学
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PubMed
高影响因子
RENEWABLE ENERGY
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2022
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IF 8.634
Lijuan Su,Xiaojie Shao,Lin Chai,Hui Ge,Hongliang Wang,Xiaojing Cui,Tiansheng Deng,Xianglin Hou
A series of mesoporous solid acid catalysts (PDS-x) with large BET surface area, superior thermal stability, strong sulfonic acid groups and tunable Brønsted acidity were synthesized by the copolymerization of divinylbenzene (DVB) and sodium p-styrenesulfonate (SPSS). The PDS-x catalysts showed high activity on the direct and efficient production of triacetylglycerol (TAG) via acyl exchange reaction of oils (fats) and acetic acid. The highest TAG yield of 93.0 mol% was obtained on the PDS-x catalysts at a mild condition of 200 °C. By combining SEM, TEM, FT-IR/DRIFTS, BET, XRD , XPS , EA, 31 P MAS NMR and TG-DTG, the key factors that affected the TAG yield were clarified on the PDS-x catalysts. Moreover, the origin of the slow deactivation on these catalysts was elucidated. The large BET surface area and abundant mesopores of catalysts allowed the contact of large-sized oils (fats) with the strong sulfonic acid groups, accounting for the high TAG yield.
研究领域:
化学工程
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催化材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 13.2
Akkammagari Putta Rangappa,Wei Xiong,Wenhua Xue,Xinxin Lu,Yiqi Geng,Yuchao Shao,Guohan Sun,Jun Zhao
Activation of molecular O 2 on catalytic surfaces to form reactive oxygen species (ROS) is a pivotal step in catalytic reactions. In this study, we synthesized a bimetallic Zn 3 In 2 S₆ (ZIS) catalyst enriched with Pd S interfaces via a straightforward cation exchange process between Pd 2+ and Zn 2+ . These interfaces function as electron reservoirs, and Pd incorporation significantly enhances photocatalytic performance by reorganizing the electronic structure of the ZIS matrix, thereby improving charge carrier dynamics and reaction kinetics. Additionally, Pd modification optimizes O 2 adsorption strength, preventing excessive population of the π* antibonding orbital that can lead to O O bond cleavage and reduce ROS generation. Theoretical calculations reveal that monodentate adsorption of O 2 on Pd-ZIS surfaces promotes efficient photo induced electron transfer across all excited states, enabling effective ROS activation. The combination of experimental findings and theoretical analysis identified the mechanisms underlying the improved selectivity of Pd-modified ZIS catalysts. As a result, the optimized Pd-ZIS-5 photocatalyst demonstrates a high photo-oxidation performance for HMF oxidation, achieving 92.4 % conversion, 86.3 % yield, and 93.4 % selectivity–representing a 1.7-fold improvement over prismatic ZIS. Overall, this work demonstrates how Pd doping and tailored O 2 adsorption strength enhance photocatalytic processes, offering valuable insights for advanced biomass conversion and sustainable chemical production.
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高影响因子
ENVIRONMENTAL RESEARCH
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2026
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IF 8.2
Zhouxiao Zhai,Jingce Bi,Linshan Wang,Ningning Liu,Yi Wang,Xia Zhang,Zhuopeng Wang,Yide Han
Mesoporous molecular sieve-supported metals have been widely investigated as catalysts for the removal of tetracycline (TC) from water via a “preconcentration-activation-degradation” catalytic system. However, the design and construction of bimetallic catalysts supported on MCM-41 for TC degradation remains a challeng. In this study, highly dispersed Al-Fe 3 N species within MCM-41(Al-Fe 3 N/Al-MCM-41) was successfully prepared, where Al originates from Al-MCM-41 subjected to high-temperature dealumination. In the presence of Al-Fe 3 N/Al-MCM-41 and PDS, 98.5% of TC was efficiently degraded within 60 min. The corresponding reaction rate constant (0.07262 min −1 ) was 2.92 times that of Fe 3 N/MCM-41 (0.02486 min −1 ). The excellent degradation performance is attributed to the enhanced electron cloud density of Fe induced by Al doping, thereby enhancing the activation efficiency of peroxydisulfate (PDS). At the same time, micro–mesoporous structure in Al-Fe 3 N/Al-MCM-41 is beneficial to preconcentration of target contaminants for the enhancement of degradation efficiency. In addition, the disinfection performance of Al-Fe 3 N/Al-MCM-41 system against antibiotic-resistant bacteria and its device-level application were explored. This work provides a novel strategy to fabricate MCM-41 with doping Fe 3 N species for the water treatment. This strategy provides a new perspective for the rational utilization of Al atoms via high-temperature dealumination method.
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Fuwei Sun,Tianhu Chen,Haibo Liu,Xuehua Zou,Peixun Zhai,Ziyang Chu,Daobing Shu,Hanlin Wang,Dong Chen
Occurring naturally siderite (FeCO 3 ) was used as the heterogeneous catalyst to activate peroxodisulfate (PDS) for the degradation of sulfadiazine under different initial pH values. The findings of this system exhibited various ROS (e.g. 1 O 2 , SO 4 − and OH) present during a wide range of pH values. Among them, 1 O 2 could significantly facilitate the initial degradation rate, and the increased pH enhanced the role of 1 O 2 . The factors including initial pH values, siderite dosage, PDS concentration, initial contaminants concentration, and water matrix were discussed. The role of each ROS was investigated through quenching test and electron paramagnetic resonance (EPR). Furthermore, the comprehensive degradation process was proposed based on the LC-MS results. And the cycle test demonstrates the reusability of siderite at a pH of 3. Accordingly, this study is of great significance for understanding the degradation of such sulfonamide pollutants in the siderite/PDS system.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ruijie Xie,Jianping Cao,Xiaowen Xie,Dongxue Lei,Kaiheng Guo,Hong Liu,Yuxuan Zeng,Haibao Huang
Chlorobenzene is a typical chlorinated volatile organic compound (CVOC), and the degradation of chlorobenzene frequently produces high-toxic byproducts such as dioxins in the treatment process. To prevent this, complete oxidation of chlorobenzene into harmless CO 2 is highly desirable. Wet scrubber coupled with advanced oxidation processes (AOPs) for gaseous VOCs treatment has been widely reported, but their mineralization capacity and mechanism are still poorly understood. Herein, this study developed an efficient technology for chlorobenzene oxidation via wet scrubbing process coupled with UV/peroxydisulfate (PDS), with UV/H 2 O 2 as comparison. The mineralization efficiency of chlorobenzene was much higher in UV/PDS (75.4%) than that in UV/H 2 O 2 (42.0%), although the removal efficiencies in both AOPs were similar at 90–97%. Sulfate radical (SO 4 •− ) was predominant for the initial oxidation of chlorobenzene, forming the intermediates that were favorable for the mineralization process. Then, O 2 and HO • played important roles on the formation of CO 2 in the complete oxidation of chlorobenzene in UV/PDS. The role of O 2 was further comfirmed by the result that high-toxic dimeric products, rather than CO 2 , were generated in UV/PDS in the absence of O 2 . The possible pathway on chlorobenzene oxidation was proposed based on the evolution of intermediates and Density Functional Theory (DFT) calculation. Carbon cation radical was formed from the initial oxidation of chlorobenzene by SO 4 •− , followed by the ring-opening and more CO 2 yields via the synergetic effect of SO 4 •− , O 2 and HO • . This study not only provides an environment-friendly method to improve the VOC removal efficiency, but also gets a deep understanding of the different functions of SO 4 •− , HO • and O 2 on the mineralization process.
研究领域:
环境科学
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化学工程
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ning Deng,Huichao Zhu,Zhiheng Fan,Changjin Guo,Jie Hu,Xin Huang
Phosphate recovery presents an effective solution to address the conflicting problems of phosphorus pollution and scarcity. However, recovering organic phosphates, such as 1-hydroxyethane 1,1-diphosphonic acid (HEDP), is comparatively complex, which involves multiple processes. Herein, we developed an innovative all-in-one solution to simplify these processes by combining NiFe-layered double hydroxides (NiFe-LDH) and peroxydisulfate (PDS). This combination achieved approximately 90 % conversion of HEDP to orthophosphate, with 100 % of the resulting orthophosphate recovered in 120 min. The exceptional performance in simultaneous HEDP degradation and recovery can be attributed to dual roles of Ni and Fe in NiFe-LDH/PDS. The polyvalent Ni functions as an electron shutter (Ni 2+ ⇋ Ni 3+ ⇋ Ni 2+ ) in the redox cycles between PDS and HEDP, accounting for effective HEDP degradation. The high complexation stability between Fe(Ⅲ) and orthophosphate (log K = 9.92) allows Fe(Ⅲ) to serve as binding sites for orthophosphate recovery. Moreover, NiFe-LDH/PDS effectively treats HEDP across wide pH ranges (3–––10), which can be ascribed to pH buffers originating from protonation/deprotonation in NiFe-LDH layers. The recovered phosphorus with NiFe-LDH exhibited a slow-release property under soil water solution without notable Ni release, which highlighted its potential usage as a slow-release fertilizer. These features—catalytic and binding sites, and high compatibility—allow NiFe-LDH to achieve concurrent degradation and recovery of organic phosphate in a single solution.
研究领域:
环境科学
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化学工程
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高影响因子
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