CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yuxiang Yang,Xiaocui Huang,Mengyang Dong,Ziling Chang,Hongming Yuan,Yan Huang,Xiangnong Liu,Jianbo Zhang,Anbang Dai
As a common pollutant in the environment, trichloroacetic acid (TCA) is difficult to be completely degraded by common advanced oxidation processes (AOPs) due to its high C-Cl bond content. Advanced oxidation–reduction processes (AORPs) may improve the degradation performance of TCA. In this work, we use Fe 0 Ni 0 bimetal as reducing catalyst, hollow mesoporous silicone nanoparticles (HMONs) modified by ZIF-8 as immobilized carrier, horseradish peroxidase (HRP) and Fe 0 Ni 0 were fixed in the carrier to form a AORP system for degradation of TCA. The effects of temperature, pH, H 2 O 2 concentration, doping ratio on the degradation performance of the catalyst and the degradation mechanism of the composite catalyst were investigated. Degradation experiments showed that H· and OH· were present in the dual system, dechlorination and decarboxylation exist at the same time. Under the condition of 55 °C and pH = 4, 30 mg Fe 0 Ni 0 and 20 mg immobilized enzyme shows the best degradation on TCA, and 81.48 % of 20 mg·L −1 TCA could be degraded by 2 h.
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Engineering
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2023
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IF 12.8
Ning Li,Haoxi Dai,Mengting He,Jun Wang,Zhanjun Cheng,Beibei Yan,Wenchao Peng,Guanyi Chen
The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate (PMS) activation and contaminants degradation. Herein, atomic layer deposition is applied to prepare Cu single atom (SA-Cu), cluster (C-Cu), and film (F-Cu) decorated MXene catalysts by regulating the number of deposition cycles. In comparison with SA-Cu-MXene (adsorption energy ( E ads ) = −4.236 eV) and F-Cu-MXene ( E ads = −3.548 eV), PMS is shown to adsorb preferably on the C-Cu-MXene surface for activation ( E ads = −5.435 eV), realizing higher utilization efficiency. More SO 4 − · are generated in C-Cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-Cu-MXene and F-Cu-MXene activated PMS systems. Particularly, the contribution of SO 4 − · oxidation to sulfamethoxazole (SMX) degradation followed the order, C-Cu-MXene (97.3%) > SA-Cu-MXene (90.4%) > F-Cu-MXene (71.9%), realizing the larger SMX degradation rate in the C-Cu-MXene/PMS system with the degradation rate constants ( k ) at 0.0485 min −1 . Additionally, SMX degradation routes in C-Cu-MXene/PMS system are found with fewer toxic intermediates. Through this work, we highlighted the importance of guided design of heterogeneous catalysts in the PMS system. Appropriate metal distribution patterns need to be selected according to the actual water treatment demand. Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.
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Alexandria Engineering Journal
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2023
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IF 6.8
Changbiao Chi,Buqing Huo,Zedong Liang,Chenxi Hu,Qingyue Sun,Shufeng Zhou
The presence of antibiotics in wastewater has become a significant concern due to their potential environmental impact and contribution to antibiotic resistance. In this study, we investigated the degradation of tetracycline, a commonly used antibiotic, in wastewater using a system based on zero-valent nano iron assisted micro-nano bubbles (MB/nZVI). The synthesized nZVI-BC composite, consisting of nano zero-valent iron particles loaded onto phosphoric acid-activated biochar, served as an efficient adsorbent for tetracycline removal. Our findings revealed that the combination of MBs and nZVI significantly enhanced the degradation efficiency of tetracycline. The MB/nZVI system exhibited the highest removal rate of 82.81% after a 2 h reaction, surpassing the performance of MB alone, nZVI-BC alone, and conventional bubble (CB)/nZVI-BC systems. Furthermore, the MB/nZVI system showed superior degradation performance at a dosage of 25 g/L and an MB flow rate of 30 mL/min. The pH condition had no significant effect on tetracycline degradation in the MB/nZVI system. Our results demonstrate that the use of MB/nZVI has the potential to be a sustainable and efficient approach for the remediation of tetracycline-contaminated wastewater.
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CHEMOSPHERE
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2023
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IF 8.8
Jie Tian,Yumeng Qi,Junyan Wei,Ahmed Rady,Saleh Maodaa,Ahmed A. Allam,Zunyao Wang,Ruijuan Qu
The degradation process of bisphenol S (BPS) in ozone/peroxymonosulfate (O 3 /PMS) system was systematically explored. The results showed that the removal efficiency of BPS by O 3 could be significantly improved with addition of PMS. Compared with ozonation alone, the pseudo-first-order constant ( k obs ) was increased by 2–5 times after adding 400 μM PMS. In O 3 /PMS system, accelerated removal of BPS was observed under neutral and alkaline conditions. The removal efficiency of BPS reached 100% after 40 s of reaction at pH 7.0, with the k obs of 0.098 s −1 . Moreover, Cu 2+ had a catalytic effect on the O 3 /PMS system, because it could catalyze the decomposition of ozone and PMS to produce •OH and SO 4 •- , respectively. Electron paramagnetic resonance illustrated that •OH and SO 4 •- were the reactive species in O 3 /PMS system. Twelve intermediates were identified by mass spectrometry, and the degradation reactions in O 3 /PMS system mainly included hydroxylation, sulfate addition, polymerization and β-scission. Finally, the toxicity of the products was evaluated by the EOCSAR program. Our results introduce an efficient method for BPS removal and would provide some guidance for the development of O 3 -based advanced oxidation technology .
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
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IF 5.8
Bao Siqi,Yu Xiaotong,Li Xiaolin
Antibiotic contamination has a significant negative impact on China, one of the largest producers and consumers of antibiotics worldwide. In this study, a three-dimensional flower-like structure of CoFe-LDHs was used to efficiently degrade tetracycline (TC) in a system triggered by peroxymonosulfate (PMS) and exposed to visible light. After exploring the effects of different metal ratios, catalyst dosage, initial TC concentrations, and pH, the optimal reaction conditions were determined. In comparison to pure CoFe-LDHs, the TC elimination rate was dramatically increased by the addition of the PMS. The strong environmental resistance, excellent stability and reusability, and universal flexibility were shown. The quenching experiments and electron spin resonance detection showed that the creation of reactive oxygen species was facilitated by the synergistic transmission of electrons between the active bimetallic components. Further, photogenerated holes was the dominant oxidizing species, which contributed more to the degradation of TC. The potential degradation pathways and intermediate toxicity of TC were suggested. This work offers a new method dominated by photogenerated holes for efficiently removing TC effluent.
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PubMed
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yanan Dong,Dong Wang,Yingchen Zhu,Qianwen Wang,Guocheng Liu,Qinghua Yan,Yucan Liu,Qinghua Chen,Dong Ma,Guangshan Zhang,Shuaishuai Xin,Yanjun Xin
The self-sufficient heterogeneous photo-Fenton (SH-PF) system was constructed for doxycycline hydrochloride (DOH) degradation with hydroxyapatite (Hap) modified CuFeO 2 (Hap/CuFeO 2 ) composites through H 2 O 2 in-situ production. The modification of Hap could improve the specific surface area, visible-light response, light conversion efficiency, photoelectron lifetime and oxygen vacancies (OVs) of CuFeO 2 , which was conducive to H 2 O 2 production and DOH degradation in SH-PF system. Notably, Hap/CuFeO 2 fabricated with 0.5 g Hap (Hap/CuFeO 2 -0.5) displayed more superior performance for DOH degradation compared to other synthesized catalysts. The Hap/CuFeO 2 -0.5 load and initial solution pH for DOH degradation in SH-PF system were optimized, and the Hap/CuFeO 2 -0.5 had good reusability and stability. The • OH was the main active species for DOH degradation, and the facilitation effect of • O 2 – and photoelectrons on DOH degradation was associated with the H 2 O 2 production in the present work. In addition, the capture of photogenerated holes suppressed the recombination of photogenerated carriers, elevating the production of photoelectrons and thereby enhancing H 2 O 2 production and DOH degradation. The degradation pathways for DOH were proposed and the comprehensive toxicities of DOH were relieved after degradation in SH-PF system.
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ACS Nano
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2016
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IF 13.334
Xuning Li,Zhimin Ao,Jiayi Liu,Hongqi Sun,Alexandre I. Rykov,Junhu Wang
Innovation in transition-metal nitride (TMN) preparation is highly desired for realization of various functionalities. Herein, series of graphene-encapsulated TMNs (FexMn6–xCo4–N@C) with well-controlled morphology have been synthesized through topotactic transformation of metal–organic frameworks in an N2 atmosphere. The as-synthesized FexMn6–xCo4–N@C nanodices were systematically characterized and functionalized as Fenton-like catalysts for catalytic bisphenol A (BPA) oxidation by activation of peroxymonosulfate (PMS). The catalytic performance of FexMn6–xCo4–N@C was found to be largely enhanced with increasing Mn content. Theoretical calculations illustrated that the dramatically reduced adsorption energy and facilitated electron transfer for PMS activation catalyzed by Mn4N are the main factors for the excellent activity. Both sulfate and hydroxyl radicals were identified during the PMS activation, and the BPA degradation pathway mainly through hydroxylation, oxidation, and decarboxylation was investigated. Based on the systematic characterization of the catalyst before and after the reaction, the overall PMS activation mechanism over FexMn6–xCo4–N@C was proposed. This study details the insights into versatile TMNs for sustainable remediation by activation of PMS.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Wenjing Ren,Junkuo Gao,Chao Lei,Yuanbo Xie,Yurong Cai,Qingqing Ni,Juming Yao
Metal-organic frameworks (MOFs) as catalysts for the activation of peroxymonosulfate (PMS) to remove recalcitrant organic contaminants has been well reported, however, the separation of MOFs from the solution is difficult because of their powder state, which limits their applications. In the present study, zeolitic imidazole framework (ZIF) materials, ZIF-9 and ZIF-12 were pioneered to load on cellulose aerogels, and the hybrid aerogels as metal catalysts to effectively activate PMS for Rhodamine B (RB), tetracycline hydrochloride (TC) and p-nitrophenol (PNP) degradation. The hybrid aerogels/PMS system could remove PNP about 90% in 1 h, which hard to remove from water. The pH value of the solution had no effect on the degradation process, which demonstrated that the hybrid aerogels had excellent pH tolerance. In addition, the mechanism of PNP degradation was investigated by electron paramagnetic resonance (EPR) and free radical trapping methods. The results showed that PMS could effectively activate by hybrid aerogels to produce sulfate radicals (SO 4 −), hydroxyl radicals ( OH), and revealed that SO 4 − play a key role in degradation. The most important feature of hybrid aerogels is can be easily separated from the solution. The obtained results showed that the hybrid aerogels exhibit excellent recyclability, with no significant effect on degradation. The prepared hybrid aerogels are green, environmentally friendly with high catalytic efficiency. Further, the outstanding degradation of PNP demonstrates the promising prospects of hybrid aerogels as advanced oxidation process (AOP) catalysts.
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Journal of Physical Chemistry C
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2022
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IF 4.177
Yue-Hua Li,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Coupling photocatalytic hydrogen (H2) evolution with selective organic synthesis in one redox cycle showcases great potential for the coinstantaneous utilization of photoexcited electrons and holes toward sustainable production of value-added fuels and chemicals. Herein, we construct one-dimensional/two-dimensional (1D/2D) WO3/ZnIn2S4 (WO3/ZIS) hierarchical Z-scheme composites for bifunctional integrated light-driven H2 production and biomass-derived aromatic alcohol conversion. The superior photoactivity and selectivity over WO3/ZIS composites compared with that over bare WO3 nanorods (NRs) and ZIS nanosheets (NSs) can be attributed to the assembly of the Z-scheme heterostructure. The construction of WO3/ZIS direct Z-scheme composites not only facilitates the charge separation dynamics by transporting photoinduced electrons and holes to spatially separated redox sites but also steers the selectivity of targeted products by tuning the energy band potentials to endow electrons and holes with stronger reduction and oxidation abilities. The mechanistic studies combining the control experiments and electron paramagnetic resonance spectroscopy validate the free radical mechanism of the benzyl alcohol photooxidation reaction. It is anticipated that this work would offer a conducive paradigm for the ingenious design of high-performance Z-scheme heterostructured catalysts toward the solar light-driven collaborative redox of H2 production and selective organic synthesis.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Mantang Chen,Zhimin Zhang,Lihua Zhu,Nan Wang,Heqing Tang
The present work aimed at using bisulfites (HSO 3 − ) to enhance the oxidative degradation of bisphenol A (BPA) in a Fenton process based on the Fe 3+ -H 2 O 2 reagents. It was confirmed that both the degradation and mineralization of BPA were drastically enhanced by the addition of HSO 3 − . Typically, the use of 0.1 mmol L −1 Fe 3+ , 0.3 mmol L −1 HSO 3 − and 10 mmol L −1 H 2 O 2 achieved a complete degradation of BPA (0.05 mmol L −1 ) in only 2 min. The addition of HSO 3 − increased the BPA degradation rate constant from 0.045 min −1 in the Fe 3+ -H 2 O 2 system to 2.71 min −1 in the Fe 3+ -HSO 3 − -H 2 O 2 system by 60 times. This drastic enhancement effect of HSO 3 − was attributed to its complexing and reducing abilities. The formation of FeSO 3 + complex prevented the precipitation of Fe 3+ and accelerated the cycling of Fe 3+ /Fe 2+ ; the reducing ability of HSO 3 − further favored the transformation of Fe 3+ to Fe 2+ . Several reactive species, including OH, SO 3 − and SO 4 − were responsible for the degradation of BPA, among which OH was the dominant one. The proposed Fe 3+ -HSO 3 − -H 2 O 2 system is suggested be able to act as the followed stage of a traditional Fe 2+ -H 2 O 2 system in the engineering setting.
研究领域:
环境科学
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化学工程
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污染控制
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Zhao Mu,Shu Wu,Jingjing Guo,Min Zhao,Yan Wang
The study of the mechanism of peroxidase-like activity of nanozymes, to obtain high-performance, is of great significance in biosensing and biocatalysis. Herein, the developed bimetal–organic frameworks (FexNiy-MOF) all showed enhanced peroxidase-like activity, and the research was carried out on behalf of Fe3Ni-MOF with the best catalytic activity. The dual mechanism (electron transfer mechanism and generation of hydroxyl radicals (•OH) mechanism) of the enhanced peroxidase-like activity of Fe3Ni-MOF was deduced through the cyclic voltammetry and electron spin resonance. The enhanced peroxidase-like activity mainly depends on the introduction of Ni, which improved the redox capacity of Fe3Ni-MOF and accelerated the electron transfer between TMB and H2O2. In addition, the introduction of Ni also improved the conversion efficiency between Fe3+ and Fe2+, to promote the generation of •OH, and then enhanced the peroxidase-like activity. The Fe3Ni-MOF we obtained can achieve ultrasensitive detection of H2O2 with a linear range of 0.02–15 μM and a detection limit as low as 11 nM. This makes the enhancement of peroxidase-like activity of practical significance. Then, a glucose detection system was successfully established with using H2O2 as an intermediate product, which has great potential in the development of biosensor applications.
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CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Jing-Yu Li,Ming-Yu Qi,Yi-Jun Xu
Integrating selective organic synthesis with hydrogen (H 2 ) evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals. In this work, a facile one-pot oil bath method has been proposed to fabricate a noble metal-free ultrathin Ni-doped ZnIn 2 S 4 (ZIS/Ni) composite nanosheet for effective solar-driven selective dehydrocoupling of benzyl alcohol into value-added C–C coupled hydrobenzoin and H 2 fuel, which exhibits higher performance than pure ZIS nanosheet. The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position, which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer. Furthermore, it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products. It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.
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