CHEMOSPHERE
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2022
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IF 8.943
Lu Zheng,Yifan Gu,Baolv Hua,Jiarui Fu,Fengting Li
Metal-organic frameworks have been investigated in Fenton-like catalysis for tetracycline hydrochloride degradation, a widely used antibiotic which threatens the growth and health of creatures. However, powder phase and absence of large pores limit the materials’ degradation performance and application. In this work, a hierarchical macro-meso-microporous composite melamine sponge@MIL-101-Fe-NH 2 was firstly designed and constructed. While the micropores provided plenty of active sites to generate reactive oxygen species , the macropores and mesopores accelerated mass transfer. Besides, MIL-101-Fe-NH 2 particles dispersed on melamine sponge individually, exposing more catalytic sites and avoiding inactivation caused by aggregation compared to powder catalysts. Its catalysis performance for tetracycline hydrochloride degradation was evaluated through changing various influence factors like H 2 O 2 concentration, catalyst amount, pH and coexisting ions. Different from the preference of homogenous Fenton catalysts for pH 2–4, the composite displayed the most effective degradation at a subacid environment closer to nature with 77.24% in 30 min. Owing to the synergistic effect of hierarchical porous structure and monodispersed nanoparticles , the composite exhibited faster reaction rate and longer persistence compared to powder MIL-101-Fe-NH 2 . Easy recycling and less ion leaching made it advantages for practical application. •OH, •O 2 − and 1 O 2 active species contributed together to the degradation and two main possible degradation pathways were put forward based on 35 detected intermediates.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2022
·Vol. 26
·期 10
·2231-2246
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IF 2.747
Wang Li,Wang Junbo,Yu Aishui,Yu Zuolong
In this paper, removal of malachite green (MG) by two separate processes, namely electrochemical oxidization polymerization and electrochemical reduction precipitation process, was studied. Reaction rate constants ( k 0 ), exchange current density i 0 , the transfer coefficients β and the diffusion coefficient D values were all tested. TR-FTIR (time-resolved Fourier transform infrared spectroscopy), UPLC-MS (ultra-performance liquid chromatography–mass spectrometry), and GC–MS (gas chromatography–mass spectrometer) analyses were applied to investigate the pathway and mechanism of MG degradation. The results show that both electrochemical oxidization polymerization and electrochemical reduction precipitation process were efficient to remove MG.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Junhua Li,Linsen Huang,Zhimei Yang,Zengjian Liu,Xiaosong Sun
Sunlight driven photocatalytic degradation is an effective and eco-friendly technology for water remediation . And formation of metal-semiconductor heterojunction provides a promising strategy to enhance the photocatalytic efficiency of photocatalyst. In this work, the hierarchical Cu 2 O/Cu hollow sphere was newly prepared by a simple template-free and one-pot solvothermal method without using any organic capping agents. The composition, morphology structure and photoelectric properties of the prepared photocatalysts were investigated by the characterization of XRD, XPS, SEM, TEM , nitrogen adsorption/desorption isotherms, UV-DRS and EIS, etc. It was found that the Cu 2 O/Cu composite with hierarchical hollow sphere structure exhibits good stability and excellent photocatalytic activity for the degradation of methyl orange (MO) and tetracycline (TC) under visible light, because the huge specific surface area provides more active sites and the Cu 2 O/Cu heterojunction could efficiently facilitate photogenerated carries separation. Further, free radical scavenging experiments and EPR tests confirmed the ·O 2 - radicals were produced and played the most important role in the photocatalytic process. Finally, the possible photocatalytic mechanism and the transfer processes of photogenerated carriers of hierarchical Cu 2 O/Cu hollow sphere was proposed. As a result, the hierarchical Cu 2 O/Cu hollow sphere may be a suitable candidate of high-efficiency photocatalyst for the wastewater treatment .
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WATER RESEARCH
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2022
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IF 13.4
Yumeng Zhao,Yanxin Zhao,Xin Yu,Dezhen Kong,Xinru Fan,Runzhi Wang,Shuangjiang Luo,Dongwei Lu,Jun Nan,Jun Ma
Endowing ceramic membrane (CM) catalytic reactivity can enhance membrane fouling control in the aid of in situ oxidation process. Peracetic acid (PAA) oxidant holds great prospect to integrate with CM for membrane fouling control, owing to the prominent advantages of high oxidation efficacy and easy activation. Herein, this study, for the first time, presented a PAA/CM catalytic filtration system achieving highly-efficient protein fouling alleviation. A FeOCl functionalized CM (FeOCl-CM) was synthesized, possessing high hydrophilicity, low surface roughness, and highly-efficient activation towards PAA oxidation. Using bovine serum albumin (BSA) as the model protein foulant, the PAA/FeOCl-CM catalytic filtration notably alleviated fouling occurring in both membrane pores and surface, and halved the flux reduction degree as compared with the conventional CM filtration. The PAA/FeOCl-CM catalytic oxidation allows quick and complete disintegration of BSA particles, via the breakage of the amide I and II bands and the ring opening of the aromatic amino acids (e.g., Tryptophan, Tyrosine). In-depth investigation revealed that the in situ generated • OH and 1 O 2 were the key reactive species towards BSA degradation during catalytic filtration, while the organic radical oxidation and the direct electron transfer pathway from BSA to PAA via FeOCl-CM played minor roles. Overall, our findings highlight a new PAA/CM catalytic filtration strategy for achieving highly-efficient membrane fouling control and provide an understanding of the integrated PAA catalytic oxidation - membrane filtration behaviors.
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COMPOSITES PART B-ENGINEERING
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2022
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IF 11.322
Yang Wang,Jiawen Yang,Xiru Qin,Jiayi Zhuang,Wujie Yin,Tingting Chen,Yong Yao
Simultaneous using photogenerated electrons and holes in one reaction to produce H 2 and value-added organic intermediates hold great promise for the green synthesis of chemicals and clean energy. Herein, we designed an efficient, noble-metal free and dual-photocatalyst Ni/Zn 3 In 2 S 6 for simultaneous aldehydes synthesis and H 2 production under visible light irradiation. Due to the reasonable band structure of Zn 3 In 2 S 6 and the Schottky barrier established between Zn 3 In 2 S 6 and Ni, the photogenerated electrons and holes with suitable redox potentials can be spatially separated and efficiently transferred. Thereby, alcohols can be highly selective oxidized into corresponding aldehydes or carbonyl compounds at Zn 3 In 2 S 6 by the holes, and the released protons can be rapidly reduced into H 2 at Ni by the electrons. The H 2 evolution of the optimal Ni/Zn 3 In 2 S 6 can reach up to 277.2 μmol h −1 , which is about 6.5 and 5.3 times as high as that of the pristine Zn 3 In 2 S 6 and the Pt/Zn 3 In 2 S 6 , respectively. Ni/Zn 3 In 2 S 6 also shows the stability and general applicability for other aromatic and non-aromatic alcohols. Compared with NiS x , NiO x and Ni 2+ cocatalysts , the metallic state of Ni is the key to achieving these photoredox reactions for effective utilization of photoexcited holes and electrons in one reaction system. During the photoredox reactions, two protons derived from O –H and Cα-H are abstracted from alcohols and then reduced into H 2 by the photogenerated electrons. At the same time, alcohols are oxidized into aldehydes or carbonyl compounds by the photogenerated holes.
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BIORESOURCE TECHNOLOGY
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2022
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IF 11.889
Qinyang Li,Yuling Tang,Bo Zhou,Jianfei Zhou,Bi Shi
In this work, a low-cost carbon-based catalyst (TSBC) was prepared by the facile one-pot pyrolysis of tannery sludge (TS) and used to activate persulfate (PS) for tetracycline (TC) removal. The results showed that TSBC-500 exhibited optimal physicochemical properties and the best performance for PS activation to remove TC from drinking water. Approximately 99.1% of TC was removed in the TSBC-500/PS system, which was considerably higher than those in the TSBC-500 adsorption and pure PS systems. Radical quenching experiments indicated that •OH and SO 4 • - played major roles in the TC removal in the TSBC-500/PS system. In addition, transition metals, functional groups, and the high degree of carbon structural defects were beneficial for PS activation to degrade TC. This study not only newly contributes to high-value utilization of TS as a PS activator but also offers an efficient method for the removal of organic pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mengmeng Lou,Xiaowei Zhu,Xiaofeng Fang,Yanbiao Liu,Fang Li
The unimpeded transport of volatile organic compounds (VOCs) in the membrane distillation (MD) greatly restricts its application in treating industrial wastewater treatment. Herein, an electrically MD process (E-MD) was conducted by coupling electrified carbon nanotube (CNT) membrane for the VOCs intercept test. This work systematically investigated membrane characteristic, the intercept efficiency and mechanism of VOCs in the E-MD. The results showed that CNT significantly promoted conductivity and permeate performance of the membrane. The transport of 7 VOCs across the membrane was highly correlated with their molecular weights and hydrophobicity. By applying a low voltage of 3.0 V on the membrane surface, the distilled VOCs concentrations were efficaciously reduced. Meanwhile, the distilled phenol concentration was only 0.15 mg/L in the E-MD, 62 times lower than that in standard MD. Moreover, the cathodic CNT and anodic CNT modes were adopted, which exhibited different intercept efficiencies. Compared with the cathodic CNT, the anodic CNT mode was superior in intercepting VOCs but with poor stability due to electrochemical byproducts induced CNT fouling. As revealed by mechanism investigation, direct electrooxidation and electropolymerization contributed to the VOCs intercept under the anodic CNT mode. By contrast, the favorable intercept efficiency under the cathodic CNT mode was mainly ascribed to the locally elevated pH near the CNT surface achieved through water electrolysis. At an elevated pH, phenol compounds were substantially ionized, and were therefore more favorably intercepted by the electronegative CNT networks of membrane surface. This study emphasizes the application potential of electrified MD membranes in reducing noxious VOCs of the cold stream.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lijun Luo,Demei Meng,Lijin He,Xiaoxia Wang,Lihong Xia,Xuejun Pan,Fengzhi Jiang,Hongbin Wang,Jianhui Dai
A new porous C 3 N 4 /reduced graphene oxide/TiO 2 nanobelt catalyst (CRT) was assembled and used to remove 17α-ethinylestradiol (EE2) in the presence of peroxydisulfate (PS) and visible light. The characterization results showed that larger porous graphite carbon nitrides (pg-C 3 N 4 ) covered onto the surface of TiO 2 /reduced graphene oxide (RGO), in which layered RGO was wrapped onto the surface of anatase TiO 2 nanobelt uniformly. The layered RGO in CRT played significant role in separation of electron-hole pairs and nonradical activation. The electron paramagnetic resonance and quenching experiment revealed that h + , 1 O 2 and •O 2 – and direct electron transfer route contributed to complete removal of 6 mg/L EE2 within 6 min only with 0.5 g/L dosage and 1 mM PS. The degradation rate of EE2 in CRT/PS/Vis was 207.51 times than that in photocatalysis. The degradation products were identified by a solid phase extraction pretreatment method combined with ultra-high-performance liquid chromatography-mass spectrometry, and possible degradation pathways were proposed. Moreover, the estrogenic activities can be rapidly eliminated in CRT/PS/Vis process.
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ACS Catalysis
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2022
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IF 13.7
Dongmiao Li,Jinni Shen,Jiangjie Zhang,Yao Chai,Yanyu Xie,Chengwei Qiu,Mengmeng Ni,Yuanhui Zheng,Xuxu Wang,Zizhong Zhang
The development of direct conversion for selective functionalization of inert methane plays an important role in the chemical sciences. Here, we report a photocatalytic approach to successfully convert methane into methyl chloride over NaTaO3 photocatalyst using an alkali chloride solution as the chlorine source under ambient conditions, which can overcome disadvantages of toxicity and corrosiveness in the traditional chlorination of methane. Various noble metals and oxide cocatalysts (Pt, Pd, Au, Ag, and Ag2O) and different chloride ion solutions (NaCl, KCl, LiCl, MgCl2, BaCl2, CaCl2, CuCl2, FeCl3, ZnCl2, etc.) are investigated to optimize the photocatalytic chlorination processes. Ag2O/NaTaO3 is the best photocatalyst, giving the maximum CH3Cl yield of 152 μmol g–1 h–1 in aqueous NaCl solutions and an apparent quantum yield of 7.2% under 254 nm monochromatic light irradiation. The target product CH3Cl is verified to be formed by a direct combination of the photoinduced species •CH3 and •Cl on the Ag2O surface. This work provides a meaningful approach for the conversion of methane into chloromethane under normal conditions.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qikai Shentu,Zenglong Wu,Wenkai Song,Shiyuan Pan,Zhenyang Zhou,Weiyang Lv,Changsheng Song,Yuyuan Yao
Developing metal-free catalysts for persulfate-mediated oxidation process has been extensively pursued in environmental remediation, yet the activity of these catalysts is typically low and the mechanism is ambiguous. Herein, a facile one-step pyrolysis method was employed to synthesize the carbon doped boron nitride (C-BN) derived from polydopamine coated BN nanosheets. The C-BN could readily activate peroxymonosulfate (PMS) with the activation energy as low as 14.95 kJ/mol, giving rise to admirable performance for bisphenol A removal even at 0 ℃, which was superior to most reported metal-free catalysts. The combined experimental and density functional theory (DFT) analyses pointed out that the remarkable performance of C-BN originated from the B-N-C moieties, which could induce the electron transfer from catalyst to PMS to promote the fast generation of superoxide radicals (O 2 •− ) as the dominant reactive species. These findings take a step toward exploring the highly efficient metal-free catalysts for realistic applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Pei Chen,Ningning Dong,Junjie Zhang,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
In this study, zinc peroxide (ZnO 2 ) with broad energy gap was firstly used for visible-light-induced photocatalytic degradation of tetracycline (TC) and inactivation of Escherichia coli ( E. coli ). A small amount of ZnO 2 (10 mg) could efficiently degrade 100 mL of 50 mg/L TC in a wide pH range (4–12), and the degradation performance was rarely suppressed by common matrix species and natural water sources. Also, 100 mg/L ZnO 2 could inactivate around 7-log E. coli cells within 60 min under visible-light irradiation. Quenching experiments and electron paramagnetic resonance (EPR) results confirmed that superoxide radical (•O 2 − ) and singlet oxygen ( 1 O 2 ) were the main reactive oxygen species (ROS), which were attributed to the self-sensitization of TC and the photoexcitation of released H 2 O 2 under the catalysis of Zn(OH) 2 from the hydrolysis of partial ZnO 2 , respectively. The pathways of TC degradation and processes of visible-light-induced TC degradation and E. coli inactivation were proposed and deduced in detail. This work presented the enhanced visible-light photocatalytic activities of ZnO 2 for antibiotic degradation and bacterial inactivation, and provided a deep insight into the mechanisms of visible-light-induced TC degradation and E. coli inactivation over ZnO 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Feifan Yu,Wenkai Song,Zenglong Wu,Wenxian Chen,Jinping Cui,Yuyuan Yao
The removal of heavy metal ions from industrial effluents by molybdenum disulphide (MoS 2 ) has attracted considerable attention, but developing the removal capacity of MoS 2 toward hexavalent chromium ions (Cr(VI)) in wastewater treatment is still a challenge. Herein, a cationic polyacrylamide aerogel (CPAMA) containing -N + (CH 3 ) 3 was creatively introduced as a precursor to synthesize the CPAMA intercalated MoS 2 (MoS 2 @CPAMA). The addition of CPAMA as carrier greatly improved the dispersion and the exposure of active sites of MoS 2 , and even the -N + (CH 3 ) 3 effectively increased the surface potential of MoS 2 , which facilitated the adsorption and reduction for Cr(VI). Notably, MoS 2 @CPAMA removed 95% of Cr(VI) within 50 min and the maximum Cr(VI) removal capacity reached 800.0 mg g −1 at 400 mg L −1 , which was significantly higher than that of MoS 2 (237.1 mg g −1 ) and almost all reported MoS 2 -based materials. The results of ICP-OES and UV–vis spectrophotometer revealed that both reduction and adsorption pathway were participated during the Cr(VI) removal process, while the reduction was obviously dominated. The results of XPS showed that the -N + (CH 3 ) 3 and amide groups played a significant role in adsorbing Cr(VI) onto the MoS 2 @CPAMA surface, and the Mo was oxidized from Mo 4+ to Mo 6+ and the S 2− was oxidized into S 6+ subsequently during the reduction of Cr(VI). Interestingly, MoS 2 @CPAMA could also be used as a co-catalyst in the Fe 2+ /PMS system, and the TOC removal rate of 67% in 60 min and the retention rate of 80% for Fe 2+ were achieved. Notably, MoS 2 @CPAMA possessed high durability in the co-existing cations and anions, and the 4-CP removal rate was still as high as 94% after four consecutive cycles, indicating the splendid reusability of MoS 2 @CPAMA. This study offers new insights into the development of multifunctional MoS 2 -based materials for wastewater treatment.
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