CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Biyang Zhu,Yifan Chen,Shiyuan Chang,Huamai Qiu,Lijun You
Kinetic models and mechanism of isomaltooligosaccharides (IMOs) by hydroxyl ( OH) radicals-driven degradation in ultraviolet/hydrogen peroxide system were investigated. Electron paramagnetic resonance spectra indicated that UV radiation played an important role in the steady generation of OH radicals. The OH radicals could effectively decrease the molecular weight of IMOs and significantly oxidize hydroxy group into carbonyl and carboxy groups . Main components of IMOs were separated and identified by HPAEC-PAD and UHPLC-MS/MS methods. Degradation behaviors of IMOs were well fitted to pseudo first-order kinetics. The hydrogen abstraction by OH radicals from different C H sites at pyranose ring began a cascade reaction leading to cleavage of α-glycosidic linkage or C C bonds with formation of stable uronic/aldonic acids. Degradation rate was closely influenced by the degree of polymerization (DP) of IMOs, the initial concentrations of IMOs and H 2 O 2 . The results would pave the way for free radicals-driven degradation of polysaccharides .
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高影响因子
ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Jinxin Li,Dan Zhong,Yiru Chen,Kefei Li,Wencheng Ma,Shaobo Zhang,Jingna Zhang,Aoshuang Sun,Haijiao Xie
Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A 2 BO 4 -type perovskite (La 2 CuO 4 ) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La 2 CuO 4 also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O 2 − and 1 O 2 in La 2 CuO 4 /H 2 O 2 system. The La 2 CuO 4 were more favorable for H 2 O 2 activation and have a lower adsorption energy than LaFeO 3 . XPS of fresh and spent La 2 CuO 4 illustrated that the decomposition of hydrogen peroxide (H 2 O 2 ) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xuefei Zhou,Jiacheng Li,Huichao Guo,Yalei Zhang,Libin Yang,Jiabin Chen
Sulfate radical-based technologies have been frequently applied to degrade pharmaceutical and personal care products (PPCPs). Metal-based catalysts have shown great potential for activating persulfate (PS) and peroxymonosulfate (PMS) to degrade PPCPs. In this study, a Ru-based perovskite (ARuO 3 , A = La, Ba, Ce, Sr) was synthesized by the sol–gel method and used as a catalyst to activate PMS for the degradation of carbamazepine (CBZ). Results demonstrated that the A-site cations had a significant influence on the catalytic performance of the perovskite, and the degradation efficiency of CBZ in descending order for different Ru-based perovskites was as follows: La > Ba > Sr > Ce. LaRuO 3 was selected as the optimal catalyst for CBZ degradation. LaRuO 3 efficiently activated PMS to degrade CBZ in a neutral environment. The reaction rate constant had a positive linear correlation with the concentration of PMS in a range between 0.1 mM and 0.5 mM. ESR analysis and radical quenching experiments confirmed the existence of 1 O 2 , •OH, and SO 4 •− in the LaRuO 3 /PMS system, and SO 4 •− played the most significant role in decomposing CBZ. The recycling experiment and XPS spectra suggested the stability of LaRuO 3 .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Meng Xie,Mingya Yao,Shiyong Zhang,Lingshuai Kong,Lingxi Zhao,Jinhua Zhan,Ru-Song Zhao
Carbon-based single-atom cobalt catalysts exhibit high catalytic activity for the removal of novel pollutants in advanced oxidation processes. Here, atomically dispersed Co species with five-coordinated nitrogen atoms on carbon nanotubes (CNT) catalyst (Co-N 5 /CNT) was successfully fabricated via a low-temperature solvothermal reaction. The obtained Co-N 5 /CNT catalyst exhibited superior catalytic performance for PMS activation for sulfamerazine degradation. Its apparent rate constant k obs was 1.6 times higher than that of the Co-N 4 /CNT catalyst with four-coordinated nitrogen atoms prepared by the same method. Electron transfer non-radical mechanism was the main pathway for Co-N 5 /CNT to activate PMS. Higher single-atom cobalt metal loading (1.39 wt% vs 1.08 wt% in Co-N 4 /CNT) and significantly enhanced electron transfer ability (0.82 e vs 0.77 e in Co-N 4 /CNT) were the key factors for its superior catalytic performance. This work demonstrates a novel carbon-based single-atom cobalt catalyst for the removal of novel antibiotic contaminants by activating PMS in environmental catalysis applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Wenjie Kuang,Zhang Yan,Jinxiu Chen,Xiaotang Ling,Wenxiao Zheng,Weijun Huang,Chunhua Feng
Electrochemical oxidation has been demonstrated to be a useful method for removing biorefractory organic pollutants in mature landfill leachate but suffers from low efficiency in eliminating ammonium because of its resistance to being oxidized by HO• or free chlorine (FC) at decreased pH. Here, we propose a new bipolar membrane-electrochlorination (BPM-EC) process to address this issue. We found that the BPM-EC system was significantly superior to both the undivided and divided reactors with monopolar membranes in terms of elevated rate of ammonium removal, attenuated generation of byproducts (e.g., nitrate and chloramines), increased Faradaic efficiency, and decreased energy consumption. Mechanistic studies revealed that the integration of BPM was helpful in creating alkaline environments in the vicinity of the anode, which facilitated production of surface-bound HO• and FC and eventually promoted in situ generation of ClO•, a crucial reactive species mainly responsible for accelerating ammonium oxidation and selective transformation to nitrogen. The efficacy of BPM-EC in treating landfill leachates with different ammonium concentrations was verified under batch and continuous-flow conditions. A kinetic model that incorporates the key parameters was developed, which can successfully predict the optimal number of BPM-EC reactors (e.g., 2 and 5 for leachates containing 589.4 ± 5.5 and 1258.1 ± 9.6 mg L–1 NH4+-N, respectively) necessary for complete removal of ammonium. These findings reveal that the BPM-EC process shows promise in treating ammonium-containing wastewater, with advantages that include effectiveness, adaptability, and flexibility.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jin-Long Zhu,Shi-Peng Chen,Wei Lin,Hua-Dong Huang,Zhong-Ming Li
It is a daunting task to balance the catalyst stability and exposure of active site of highly efficient immobilizing photocatalyst system for wastewater treatment. In this study, an in-situ mineralization method based on homogeneous system was proposed to directly construct amorphous TiO 2 into cellulose hydrogel network as the crosslinker for efficiently and safely processing wastewater. This unique structure not only endowed TiO 2 /cellulose microsphere (TMS) with an adsorption capacity of 91.7 mg/g on methylene blue, which was approximately 14 times to cellulose microsphere containing commercial TiO 2 nanoparticles, but also made TMS reusable due to its pH sensitive adsorption capacity. More interestingly, TMS exhibited an auto-accelerating process in decomposing Rhodamine B where the degradation intermediate could act as the receptor of photo-regenerated holes to improve photocatalytical activity. In further cyclic test, the degradation rate constant of intermediate-adsorbed TMS was up to 0.02 mg −1 min −1 . Moreover, the intermediate-adsorbed TMS obtained visible light responsive property, including a removal ratio of 86.3 % against tetracycline (c 0 = 20 mg/L) in 120 min. This in-situ cellulose mineralization provides a new sight into the design of hydrogel immobilized catalyst system with high dispersion and active site exposure for efficient and safe water treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhiran Hou,Wei Wang,Ningning Dong,Pei Chen,Lifa Ge,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
In this study, a dual-oxidant advanced oxidation process (AOP) system containing calcium peroxide (CaO 2 ) and peroxymonosulfate (PMS) was developed for the first time to efficiently degrade refractory organic pollutants . It was found that the system with 0.1 g/L CaO 2 and 0.3 g/L PMS could degrade more than 91% of 50 mg/L tetracycline (TC) within 4 min at room temperature, and the degradation process much followed the pseudo second-order kinetic model. The presented AOP system exhibited strong anti-interference capabilities towards coexisting inorganic anions (Cl − , SO 4 2– , NO 3 – , HCO 3 – and HPO 4 2– ) and humic acid (HA), even at high concentrations. Moreover, the system could efficiently work in a wide pH (3−12) range, suitable for natural waterbodies and various organic pollutants. The results of quenching experiments and electron paramagnetic resonance (EPR) tests demonstrated that singlet oxygen ( 1 O 2 ) was the dominate reactive oxygen species (ROS) responsible for organics degradation. A synergistic mechanism of the dual-oxidant system was confirmed by a series of comparative experiments, where CaO 2 continuously provided OH − and H 2 O 2 , and then combined with PMS to produce predominant 1 O 2 and inferior O 2 •– , respectively. Further, the possible pathways of TC degradation were deduced based on analyses of the intermediates.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Xiangyu Peng,Jiayi Tian,Shuai Zhang,Wei Xiao,Xiaozhen Tian,Yubin Wang,Juanqin Xue,Dashi Lei
Rational design of photoelectrode with high visible light utilization rate and separation efficiency of electron-hole pairs is the key step in photoelectrocatalytic technology. In this work, Z-Scheme photoelectrocatalyst (ZTO/rGO/Ag/AgBr) was synthesized by hydrothermal and photo-reduction process. Comparing with pure Zn 2 SnO 4 (ZTO), adding reduced graphene oxide (rGO) effectively improved electrons transfer efficiency. Notably, the addition of Ag/AgBr not only broaden the visible light response range of ZTO, but also accelerated the separation of photo-generated electron-hole pairs, and constructed all-solid-state Z-Scheme heterojunction . Meanwhile, DFT calculation showed that Ag metal on rGO surface could act as active site for organic dyes degradation . Moreover, the addition of extra bias potential during photoelectrochemical process not only accelerate the migration of carriers, but also inhibit the recombination of photo-generated electron-hole pairs. Methylene blue (MB) could be effectively removed during photoelectrochemical reaction process, which was attributed to hydroxyl radical (•OH) and superoxide radical (•O 2 - ). In this work, Z-Scheme transfer pathway, assisted photoelectrocatalytic technology, is a feasible strategy for improving catalytic performance.
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ENVIRONMENTAL POLLUTION
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2022
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IF 9.988
Yao Tang,Jibo Dou,Zhijiang Lu,Jianming Xu,Yan He
The sluggish Fe 3+ /Fe 2+ cycle was the rate-limiting step in the Fenton-like reaction, and metal-free carbonaceous materials are considered as emerging alternatives to solve this problem. However, the effect of carbon material properties on the distribution of reactive species remains poorly understood. This study investigated the possibility and mechanism of using biochar to accelerate the Fe 3+ /Fe 2+ cycle to overcome the low efficiency of Fe 3+ /persulfate (PS) catalytic oxidation of phenanthrene . More importantly, the contribution of reactive species in the reaction systems with the variation of biochar pyrolysis temperatures was quantitatively studied. The results showed that medium-temperature derived biochar (BC500) had the greatest ability to enhance the Fenton-like system compared to the low- and high-temperature (BC350/700), and the first-order rate constant achieved 5.2 and 35.7-fold increase against the biochar/PS and Fe 3+ /PS systems, respectively. Using electrochemical evidence, sulfoxide probe tests, and steady-state concentration calculations, radicals yields were found to rise and then reduce with decreasing pyrolysis temperature, while the nonradical contribution of Fe(IV) increased to 56.3%. Electron paramagnetic resonance, Boehm titration, and Raman spectroscopy unraveled that the enhanced effect of biochar resulted from itself persistent free radicals, phenolic-OH, and edge defects, which enabled electron transfer between Fe 3+ and biochar. Fe 2+ was thus continuously generated and effectively activated the PS. This work enables a better understanding of the Fe 3+ -mediated Fenton-like reaction in the presence of biochar and provides a sustainable green strategy for Fenton chemistry with potential applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yi Chen,Shuai Dong,Shiyue Wei,Shiruo Zhang,Jiaxin Zhang,Jinchuan Gu
Mesoporous sodalite (SOD) zeolite was fabricated from industrial waste lithium silica fume (LSF) through the reactive oxygen species (ROS) method under ultraviolet (UV) irradiation without the template. Persulfate (PS) and peroxymonosulfate (PMS) under UV irradiation would further induce ROS generation and result in faster crystallization to obtain highly crystalline and abundant mesopores (mesopore volume, Vmes＞0.34 cm³/g) SOD within 2 h. The ROS produced in the synthesis system were detected by electron spin resonance (EPR), and the results revealed that ·OH, O 2 · − , 1 O 2, and SO 4 · − may be related to the accelerating process. Zeolite produced superior adsorptive capacity (112.4 mg/g) and reusability in copper ion (Cu(II)) adsorptive experiments. The abundance of mesoporous in zeolite facilitates the removal of Cu(II) by ion exchange and hydroxyl complexation. This work opens up a new route for green and fast synthesis of zeolite and highly efficient Cu(II) removal adsorbent.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mengxiang Ye,Chao Zhang,Zhenzhen Liu,Huaimeng Li,Zhen Fu,Haimin Zhang,Guozhong Wang,Yunxia Zhang
Extensive utilization and excessive accumulation of bisphenol A (BPA) has posed a serious threat to the whole ecosystem, necessitating the rational design of metal-based catalysts capable of complete mineralization of BPA via electrochemical oxidation. Considering the shortage of metals resources and ever-increasing generation of electronic waste (e-waste), converting e-waste into high-performance catalysts is highly expected to offer an economical and feasible means to achieve the degradation of BPA. To this end, CuAu bimetallic catalysts are in situ electro-codeposited on the carbon cloth (CC) support with the waste central processing unit (CPU) leachate as electrolyte. Significantly, the recovered CuAu/CC composites can be directly applied as an efficient electrocatalyst for the decontamination of BPA via the electro-Fenton process. The electrocatalytic activities of the fabricated CuAu/CC electrodes can be regulated by tuning the reduction potentials during electro-deposition process. Under the optimized operational conditions, 99.5 % of BPA (50 mg/L) is removed within 120 min at a constant cathodic potential of −1.0 V (vs Ag/AgCl) in the CuAu/CC-mediated electro-Fenton system, accompanied by 64.2 % of total organic carbon (TOC) removal, highlighting a satisfactory performance of the BPA electrochemical oxidation. In addition, the proposed CuAu/CC electrode material can be facilely regenerated and reused for at least ten cycles without significant decline in BPA removal efficiency. Our work offers valuable guidance for upcycling of bimetallic alloy catalysts from e-waste and further application in electrochemical decontamination of organic pollutants, achieving the innovative target of “using waste to treat waste.”
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zhengao Wang,Guangyu Liu,Wei Chen,Lu Zhang,Zheng Qi,Guanghui Bai,Youzhun Fan,Chengli Liu,Cairong Xiao,Wei Li,Yunbing Chang,Guoyan Liang,Zhengnan Zhou,Peng Yu,Zhiguo Song,Chengyun Ning
Photo-responsive nanomaterials are promising antibiotic substitutes to treat bacterial infections. Although graphene-based two-dimensional (2D) heterojunction performs advantageous photo-excited antibacterial properties, constructing heterojunctions with matched photo-physical property is still an effective strategy for acquiring high-efficiency photo-antibacterial performance. Here, we constructed a surface plasmon resonance-enhanced graphene/bismuth oxychloride 2D heterojunction for photocatalytic antibacterial, via indirect light absorption of the heterojunction. The graphene-based 2D heterojunction displayed a bactericidal effect against S. aureus for 99.36 % under simulated sunlight irradiation for 20 min, which is much more efficient than pure BiOCl nanosheets. Furthermore, we investigated the contribution of indirect light absorption of two-dimensional heterojunction on photocatalytic antibacterial progress and found that graphene contributed 57.31 % of the antibacterial properties of heterojunction. The graphene can transfer the directly excited electrons of BiOCl semiconductor with the conjugate structure. And the enhanced photocatalytic antibacterial performance is mainly due to the surface plasmon resonance effect of graphene under irradiation of visible light, accelerating the transmission rate of photogenerated charge carriers. This study facilitated an in-depth understanding of the mechanism of visible-light-driven antibacterial and provided an ideal strategy for acquiring highly efficient photocatalytic antibacterial.
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