Catalysts
·
2023
·Vol. 13
·期 4
·715
·
IF 3.9
Dongrui Hou,Jing Luo,Qinggong Sun,Mengyang Zhang,Jianfeng Wang
In this study, Co-modified alkalinized g-C3N4(named Co-CNK-OH) was prepared for the Fenton-like photocatalytic degradation of tetracycline (TC) via a simple yet effective calcination–impregnation method. In all samples of CNK-OH with different Co2+loadings, Co-CNK-OH catalyst with the optimal content (9%) exhibited the highest catalytic activity, with 87.1% tetracycline removal and 50% removal efficiency of the total organic carbon (TOC). Mechanism studies revealed that the 9%Co-CNK-OH catalyst had the lower electrical resistance after alkalization treatment and Co2+modification, leading to a significantly accelerated interfacial charge transfer to the electron acceptor as well as effectively separating electrons and holes. The intermediates generated during the TC degradation in the photo-Fenton process were detected by HPLC-MS, which proved that the holes, superoxide radicals, and singlet oxygen are the key reactive species in the Fenton-like photocatalysis. This study provides a new option for the treatment of TC in wastewater.Keywords:Fenton-like photocatalysis;Co-CNK-OH;tetracycline;reactive oxygen species
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yanzhuo Zhang,Mengqi Xu,Shengxu Liang,Ziyan Feng,Jing Zhao
The abuse of antibiotics threatens the water environment and human health. Green treatment method is needed to degrade antibiotics such as biochar. Few studies have examined the environmentally persistent free radicals (EPFRs) and defective structure of biochar during the biochar-mediated catalytic degradation of antibiotics. In this study, biochar prepared from poplar and pine sawdust was used to activate peroxymonosulfate (PMS) to generate instant radicals (SO 4 •- and •OH) and degrade tetracycline (TC), chlortetracycline (CTC) and doxycycline (DOX). The preparation temperatures ranged from 300 °C to 900 °C. EPFRs were the main activator of PMS at 300–500 °C, and the defective structure of biochar was the main activator at 800–900 °C. The concentrations of EPFRs ranged from 1.75 × 10 18 spins/g to 6.44 × 10 18 spins/g. According to the electron paramagnetic resonance (EPR) parameter (g-factor), the main types of EPFRs were carbon-centered radicals (g 1 < 2.0030) or carbon-centered radicals with oxygen atoms (2.0030 < g 2 < 2.0040). Optimization of the degradation experiment revealed that the removal rate of antibiotics peaked when the preparation temperature was 500 °C and 900 °C. In the biochar/PMS system, the antibiotics removal rate of 90% was achieved in 40 min with an average apparent rate constant (k obs ) of 0.0588 min −1 . Analysis of the mechanism revealed that the free radical pathway (EPFRs and defective structure) can effectively activate PMS to generate SO 4 •- and •OH. However, control experiments suggested that the non-free radical pathway (singlet oxygen) had little effect on antibiotic degradation. After five cycles, the removal rate of antibiotics by biochar was still greater than 70%, indicating that biochar retains a high degradation ability. These results indicate that optimizing the preparation conditions can effectively expand the application range of the biochar/PMS system and improve the degradation of antibiotic wastewater.
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CATALYSIS LETTERS
·
2026
·Vol. 156
·期 10
·282
·
IF 2.5
Ye Qihang,Zhong Zhaoping,Yang Yuxuan,Wang Wei,Jia You,Xiong Qi,Chen Huanqi,Zheng Xiang
Furfural, a key biomass-derived platform chemical, requires efficient hydrogenation for economic and research benefits. Herein, we propose a carbon-encapsulated catalyst with optimized active sites (using carbon-containing organics) for its highly selective hydrogenation. Experimental results demonstrated that carbon loading facilitated the conversion of strong acid sites to medium‑strong acid sites on the catalyst support, and also increased the Lewis/Brønsted (L/B) ratio. Through optimization of reaction conditions and carbon loading, complete conversion of furfural and a furfuryl alcohol selectivity as high as 99.17% were achieved at 160 °C for 4 h. The prepared catalyst maintained high furfuryl alcohol selectivity even after five cycles, owing to the protective carbon layer on the active support and the well-dispersed Cu species on its surface. DFT calculations further revealed that furfural preferentially adsorbs on the catalyst surface via the η¹(O)-aldehyde configuration, confirming the promotional role of the catalyst in furfural hydrogenation. Graphical
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jialin Liang,Lei Zhang,Chengjian Li,Zhihua Mo,Maoyou Ye,Zhi Zhu,Shuiyu Sun,Jonathan W.C. Wong
Herein, a facile combination approach of chalcopyrite and sodium percarbonate (CuFeS 2 + SPC) was established to augment both TCC removal efficiency and sludge dewatering. Results showed that utilizing the CuFeS 2 dosage of 600 mg/g total solids (TS) under the optimal condition, along with the SPC dosage of 12.5 mg/g TS, an initial pH of 4.0, and a reaction duration of 40 min, led to a substantial reduction of 53.9% in the TCC content within the sludge, accompanied by a notable decrease of 36.9% in the water content. Compared to well-studied iron-based advanced oxidation processes, CuFeS 2 + SPC treatment proved to be more cost-effective and environmentally friendly. Mechanistic findings demonstrated that •OH oxidation played a significant role in TCC removal, with O 2 •− and 1 O 2 acting as secondary factors. During the CuFeS 2 + SPC process, the received •OH, O 2 •− , and 1 O 2 destroyed the main binding sites of extracellular polymeric substances to TCC, including tryptophan-like protein, amide, C O stretch, and −COO− functional groups. As a result, approximately 50% of TCC was partially degraded within the solid sludge phase after the attack of radicals. Meanwhile, the decreased macromolecular organic compounds in solid sludge attenuated the binding efficacy of TCC, giving rise to the transfer of partial TCC to the liquid phase. Ultimately, the TCC in sludge was successfully removed, and five transformation products were identified. This study significantly contributes to our understanding regarding TCC transformation and removal in the sludge conditioning process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yilan Jiang,Peifang Wang,Tingyue Chen,Keyi Gao,Yiran Xiong,Yin Lu,Dionysios D. Dionysiou,Dawei Wang
Iron-based materials are difficult to produce single oxygen ( 1 O 2 ) efficiently from H 2 O 2 . Herein, we demonstrate that 1 O 2 production from H 2 O 2 can be manipulated by regulating the lattice distortion degrees of spinel ferrite through controlling the contents of Co and Ni in Co 1−x Ni x Fe 2 O 4 . Typically, NiFe 2 O 4 , which owns the lowest lattice distortion degree, can produce 1 O 2 as the dominated reactive oxygen species with·O 2 - as the intermediate. Due to the production of 1 O 2 , the NiFe 2 O 4 /H 2 O 2 system removes bisphenol A (BPA) completely within 180 min but removes only ∼ 4% of benzoic acid . In addition, the system demonstrates significant resistance to water matrix interference, as 50 mM of Cl - , NO 3 - , H 2 PO 4 - , and humic acid inhibited the BPA degradation by only ∼0%, ∼2%, ∼40%, and ∼3%, respectively. Our work may shed light for regulating the formation of 1 O 2 from H 2 O 2 through the rational design of iron-based catalysts for Fenton-like reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Rui Liu,Mu-cheng Xu,Jin-yan Yang
Sewage disposal technology in advanced oxidation processes (AOPs) should be enriched for providing more options for practical application. Herein, degradative and mechanistic investigation of heterogeneous V 2 O 3 -activated sodium percarbonate (SPC) process was implemented in the presence of oxalic acid (OA). The experimental results indicated a strong dependency of sulfamethoxazole (SMX) degradation on SPC dosage and a wide adaptability to the ambient pH in V 2 O 3 /SPC/OA system. Efficient removal of SMX in water reached 93.4 % within 10 min at the initial presence of 0.1 g/L V 2 O 3 and 2 mM SPC. Mechanistic experiments revealed that • OH played an indispensable role in SMX degradation, which partially dominated the degradation process and partially was the main precursor of CO 3 •- and O 2 •- . Moreover, except for the single electron transfer from low-valence state of vanadium (V) species to SPC, the intramolecular electron transfer process from –OOH ligand of V complex to hydrogen peroxide (H 2 O 2 ) also participated in the generation of • OH. Additionally, the introduction of OA could provide a complex, transient acidic and reductive condition for facilitating the SMX removal process. On the other hand, the addition of OA restricted the conversion of • OH to CO 3 •- and O 2 •- . Zeolite was employed to absorb the V species in the aqueous solution after the reaction and the residual vanadium concentrations were <2 mg/L. The existence of HPO 4 2- , CO 3 2– and humic acid exerted severe inhibition on the decontamination of SMX, and F - and NO 3 – exerted slight suppression, whereas the existence of Cl - and SO 4 2- did not show conspicuous impairment. This work filled the gap of decontamination performance of SMX in vanadium based heterogenous SPC system and deepened the understanding of the application of reductant.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Yu Wang,Fengwen Yan,Jie Wu,Zhijun Huang,Liuting Song,Shunda Yuan
The utilization efficiency of single atoms is limited by the active sites being buried in support. To maximize atom utilization, Cu single atoms are anchored on the external surface of g-C 3 N 4 nanofibers (CNNFs), which are fabricated by partial thermal decomposition and subsequent self-assembly in H 2 O. The abundant N and O-containing functional groups of CNNFs are vital for the loading of Cu. Benefited from the full utilization of Cu sites, CNNF-Cu exhibits excellent Fenton-like catalytic activity for Methylene Blue degradation. The reaction kinetic constant is more than 10 times higher than that of the traditional single-atom catalyst with Cu sites evenly distributed throughout the entire support. CNNF-Cu maintains most of its catalytic activity after five cycle tests, suggesting good stability. This work provides a convenient method to maximize the utilization of single metal atoms for catalytic applications.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Yajun Tian,Chuhan Ying,Liqiu Zhang,Huimin Huang,Shuang Song,Rongwu Mei,Jun Li
Silver nanoparticles (AgNPs) and antibiotics inevitably co-exist in water environment. Nonetheless, little is known regarding the interactions between AgNPs and antibiotics or the effects of AgNPs on environmental behavior of antibiotics, particularly on sunlight-driven transformation. In the present work, we found that AgNPs obviously inhibit the photochemical decay of chlortetracycline (CTC), and CTC boosts the dissolution of AgNPs. With the help of electron paramagnetic resonance (EPR) and quenching experiment, we ascertained that these results originated from the competition between AgNPs against CTC for capturing 1 O 2 generated from CTC photosensitization. 1 O 2 reacting with CTC contributed mostly to CTC photodegradation , while 1 O 2 as well reacting with AgNPs leads to release of Ag + . When compared to reaction of 1 O 2 with CTC, 1 O 2 is prone to react with AgNPs, based on lower Gibbs free energy of AgNPs reacting with 1 O 2 . Therefore, upon CTC co-existing with AgNPs, the release of Ag + was accelerated and the photodegradation of CTC was inhibited obviously. Furthermore, the accelerated release of Ag + significantly increased their toxicity toward E. coli cells under simulate sunlight irradiation. Overall, the findings demonstrate how AgNPs interact with CTC and how these interactions affect the environmental behaviors of CTC or AgNPs, allowing more accurate assessments of the risk to ecosystems posed by AgNPs coexisting with antibiotics.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xupo Liu,Ran Wang,Mengyun Wei,Xihui Wang,Jiayao Qiu,Jingru Zhang,Shilong Li,Ye Chen
Electrochemical oxidation of biomass-based 5-hydroxymethylfurfural (HMF) is an effective approach for achieving the high-value products of 2,5-furandicarboxylic acid (FDCA). However, the restricted formation of high-valence metal active species for electrocatalysts results in a sluggish kinetic process of HMF oxidation reaction (HMFOR). Herein, we fabricated the Ni 3+ -rich cross-linked α-Ni(OH) 2 nanosheets for accelerating the HMFOR through an anion-mediated strategy. It is identified that the Cl − ions with strong penetrability replace a portion of lattice oxygen atoms in α-Ni(OH) 2 to form Ni-Cl bonds, contributing to breaking the inherent lattice order and generating a special Ni 3+ -rich structure. Owing to the promoted adsorption and accelerated oxidation of hydroxyl and aldehyde groups by the affluent Ni 3+ active species, the large oxidation current density of 116.5 mA cm −2 and HMFOR kinetic constant of 0.067 min −1 has been achieved at 1.45 V (vs. RHE). By analyzing the oxidation products, the FDCA yield and Faradic efficiency are both higher than 99.25 % and 99.36 % for five successive determinations. Therefore, this work provides an insightful anion-mediated strategy for designing high-performance electrocatalysts for biomass conversion application.
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RSC Advances
·
2023
·Vol. 13
·期 49
·34335-34347
·
IF 3.9
Yuankun Liu,Xinxia Zhang,Hongrun Liu
Iron–nitrogen co-doped modified corncob (Fe–N-BC) was synthesized using a hydrothermal and calcination method. The material shows excellent oxidation performance and environmental friendliness. When the dosage of Fe–N-BC was 0.6 g L−1, the concentration of H2O2 was 12 mM and pH was 4, ciprofloxacin (CIP) was virtually totally eliminated in 240 min under Fe–N-BC/H2O2 conditions. The TOC removal efficiency was 54.6%, and the effects of various reaction parameters on the catalytic activity of Fe–N-BC were thoroughly assessed. Through electron paramagnetic resonance (EPR) analyses and free radical quenching experiments, it was established that the reactive oxygen species (˙OH, ˙O2−, 1O2) were crucial in the elimination of CIP. Furthermore, the degradation of CIP was accelerated by the synergistic interaction between the transition metal and PFRs. A thorough evaluation was conducted to assess the respective contributions of adsorption and catalytic oxidation in the system. The degradation mechanism of CIP was proposed under Fe–N-BC/H2O2 conditions. Meanwhile, the possible degradation intermediates and pathways were proposed, and the toxicity of the degradation products of CIP was also meticulously investigated in the study. These findings offered the elimination of CIP in water a theoretical foundation and technical support.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia Wu,Ke Wang,Tianqi Yu,Shuaiqin Huang,Zhixiang Zhai,Huan Wen,Shibin Yin
The development of catalysts with high activity, selectivity, and stability is critical for biomass upgrading coupled with hydrogen evolution. In this study, we present a simple method for fabricating crystalline-amorphous phase heterostructures using the etching effect of the acidic medium generated during cobalt salt hydrolysis, resulting in the formation of NiCo(OH) x -modified Ni/NiMoO 4 nanosheets electrode (NiCo(OH) x /Ni/NiMoO 4 /NF). The nanosheets array formed during the synthesis process enlarges the surface area of the prepared catalyst, which facilitates the exposure of electrochemically active sites and improves mass transfer. Unexpectedly, the strong coupling interactions between the amorphous-crystalline heterointerface optimize the adsorption of reaction molecules and the corresponding charge transfer process, consequently boosting the catalytic activity for the 5-hydroxymethylfurfural oxidation reaction (HMFOR) and hydrogen evolution reaction (HER). Specifically, NiCo(OH) x /Ni/NiMoO 4 /NF catalyst requires only 1.34 V to obtain a current density of 10 mA cm −2 for HMFOR-coupled H 2 evolution, and operates stably for 13 consecutive cycles with good product selectivity. This work thus provides insights into the design of efficient and robust catalysts for HMFOR-assisted H 2 evolution.
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MOLECULES
·
2023
·Vol. 28
·期 23
·7906
·
IF 4.6
Rong Li,Xing Lu,Jinxiang Gao,Yifan Chen,Shunlong Pan
Peroxyacetic acid (PAA)-based advanced oxidation processes (AOPs) have attracted much attention in wastewater treatment by reason of high selectivity, long half-life reactive oxygen species (ROS), and wider applicability. In this study, cobalt ferrite (CoFe2O4) was applied to activate PAA for the removal of ofloxacin (OFX). The degradation of OFX could reach 83.0% via the CoFe2O4/PAA system under neutral conditions. The low concentration of co-existing anions and organic matter displayed negligible influence on OFX removal. The contributions of hydroxyl radicals (·OH), organic radicals (R-O·), and other reactive species to OFX degradation in CoFe2O4/PAA were systematically evaluated. Organic radicals (especially CH3C(O)OO·) and singlet oxygen (1O2) were verified to be the main reactive species leading to OFX destruction. The Co(II)/Co(III) redox cycle occurring on the surface of CoFe2O4played a significant role in PAA activation. The catalytic performance of CoFe2O4remained above 80% after five cycles. Furthermore, the ecotoxicity of OFX was reduced after treatment with the CoFe2O4/PAA system. This study will facilitate further research and development of the CoFe2O4/PAA system as a new strategy for wastewater treatment.Keywords:peroxyacetic acid;cobalt ferrite;organic radicals;singlet oxygen;fluoroquinolone antibiotics
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