SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yi Gao,Xinyang Tan,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
The water treatment performance of membrane filtration is usually restricted via the paradox between permeability and selectivity. Herein, the nitrogen doped porous carbon supported Co catalysts (CoNPC), serving as both porous filler and peroxymonosulfate (PMS) activator, were firstly filled into polyvinylidene fluoride (PVDF) matrix to construct a novel mixed matrix catalytic membrane (CoNPC@PVDF) for enhanced water purification. Owing to the robust binding between CoNPC and PVDF, a high loading (50 wt%) and even dispersion of CoNPC were realized in CoNPC@PVDF, and its permeability and selectivity were both improved with the increase of CoNPC content. The optimum CoNPC@PVDF with PMS activation assistance (FCP) exhibited effective phenol removal at short retention time (1.5 s) and high permeability (256.6 L m −2 h −1 bar −1 ). The performance of CoNPC@PVDF FCP was 2.9 and 2.5 times higher than that of filtration alone and PMS activation alone, respectively, and even dramatically outweighed the reported catalytic membranes and heterogeneous catalysts. The outstanding performance of CoNPC@PVDF catalytic membrane was mainly attributed to its thin membrane structure and high filling degree of CoNPC, resulting in ultrahigh mass transfer rate (1.8 × 10 −4 m s −1 ) and more exposed active sites for enhanced PMS activation into radicals (mainly •OH and SO 4 •− ) towards pollutant removal.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zhenfei Yang,Xinnian Xia,Ming Fang,Longlu Wang,Yutang Liu
The selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-dicarbofuran (DFF), and 2,5-furanedicarboxylic acid (FDCA) is essential to its practical application. Herein, a novel Pt/ZIS/MnO 2 (PMZIS) photocatalysts with photothermal effect were well designed for selective and controlled oxidation of HMF toward DFF or FDCA. The product distribution of HMF photo-oxidation on PMZIS can be regulated by the photothermal effect. At a low temperature (10 °C) with PMZIS, DFF is the primary oxidation product with the yield of 54.6% and selectivity of 85.4%. At a high temperature (60–70 °C) induced by photothermal effect, the FDCA can be obtained with the yield of 61.5 % and selectivity of 82.9%. Moreover, the Z-scheme transfer pathway and Pt cocatalysts realize the spatial charge separation structure of PMZIS heterojunctions. This unique structure greatly inhibits charge recombination and maximizes the activation ability of molecular oxygen to efficiently generate of the reactive oxygen species (e.g., 1O 2 and O 2– ), thus significantly improving the photocatalytic performance. This work would provide valuable insight in the product regulation through photothermal effect for the photocatalytic specific selective oxidation of organic molecules.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chaoyi Zhou,Guojun Lv,Xuyang Zou,Jiangzhang Wang,Yan Chen,Jialing Shen,Shihao Su,Weilong Xing,Deling Fan,Yangbin Shen
Room-temperature ambient air is cheap and easy to obtain, hence the application of room-temperature ambient air as sole oxidant for pollutant degradation is extremely fascinating. In this work, core–shell coordination sponge-Fe 0 @Cu-Pd trimetal catalyst was synthesized via a simple step displacement plating process employing first displacement of Cu and the subsequent displacement of Pd, and applied as heterogeneous catalyst for synergistic catalytic degradation of composite pollutants including TC and PNP. The prepared s-Fe 0 @Cu-Pd trimetal sample was characterized with XRD, SEM, TEM, VSM and XPS. The characterization results revealed the obtained s-Fe 0 @Cu-Pd trimetal sample was a 20 ∼ 30 nm core–shell spherical morphology composed of Fe 0 aggregates core wrapped by a Cu-Pd shell layer. The obtained sponge-Fe 0 @Cu-Pd trimetal catalyst could efficiently activate room-temperature dissolved ambient oxygen and achieve the largest TC removal rate of 99.08 % and PNP removal rate of 97.16 % as well as the biggest removal rate constant of 8.76 min −1 for TC degradation and 7.55 min −1 for PNP degradation within 60 min at experimental conditions: [TC] = 30 mg/L, [PNP] = 30 mg/L, [Catalyst] = 25.52 g/L, pH = 3, 298 K ascribed to the strongest oxidation and reduction ability confirmed by CV characterizations, the lowest charge transfer and contact resistance affirmed by EIS measurements, the strongest O 2 activation ability verified by O 2 -TPD characterizations and DFT analyses, the largest external surface area and mesoporous volume validated by Nitrogen adsorption and desorption characterizations as well as the synergistic catalysis effect for wrapped Cu and Pd. Quenching experiments and EPR characterizations revealed that •OH, •O 2 − , 1 O 2 and •H are all the reactive species and meanwhile •O 2 − served as the main reactive oxygen species. Furthermore, possible mechanisms of TC and PNP degradation via sponge-Fe 0 @Cu-Pd trimetal catalyst were proposed.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Mingyi Liu,Hanchun Chen,Pengfei Xiao,Haodong Ji
Copper-manganese composite metal oxides (CuMnO y ) were prepared by hydrolysis-driven oxidation-reduction method and used to activate sulfite to degrade chlortetracycline hydrochloride (CTC) for the first time. The Jahn-Teller ions Mn 3+ and Cu 2+ exist in CuMnO y , which form a solid electric charge transport redox system and ensure the continuous generation of reactive oxygen species (ROS). Through the systematic study of the experimental parameters such as sulfite concentration, catalyst metal molar ratio, catalyst amounts and initial pH, the optimal degradation rate of CTC could reach 91.74% within 10 min and 94.46% after 30 min. The major reactive radicals were determined by radical quenching experiments and electron paramagnetic resonance (EPR) trapping techniques, and it was confirmed that SO 4 •- and •O 2 - played a nonnegligible role in the process of degrading CTC. Density functional theory (DFT) calculations show that higher Fukui indices ( f - and f 0 ) of CTC sites are more vulnerable to free radical attack. CuMnO y has low CTC degradation intermediate toxicity, high catalytic performance, good anti-interference ability, reusability and stability, and possesses decent application potential in the actual water treatment field.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Aotian Gu,Chunhui Gong,Manli He,Kaiwei Chen,Xinyu Zhou,Peng Wang,Kai Chen,Yan Jiao,Yi Yang
Advanced oxidation processes activated by transition metal have attracted much attention for their excellent performance in the removal of organic pollutants , but the development of efficient and environmentally benign catalysts is still a significant challenge. In this work, carbon shell encapsulating Co/Fe sulfide nanoparticles (Co/Fe@SC X ) were synthesized by pyrolysis of the resorcinol-formaldehyde (RF) coated MIL-101 @ZIF-67 bimetal Metal-organic frameworks (MOFs). In the degradation of TCP , Co/Fe@SC 600 exhibited the highest TCP removal rate (97.33%) and reaction rate constant (k obs ) (0.169 min −1 ), as well as the mineralization rate of up to 60.19%. Compared to other prepared catalysts, Co/Fe@SC 600 not only possessed excellent catalytic activity, but also exhibited the lowest Co ion leaching concentration, good stability and high resistance to environmental factors. Further studies showed that the non-radical pathway dominated by 1 O 2 contributed most to the TCP degradation, and the radicals also played the indispensable role. The potential TCP degradation pathways in the reaction system was also investigated by analyzing the intermediate products during the degradation process. Overall, this study may provide some interesting insights into the design of advanced catalysts.
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APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Wen-Jing Yi,Yongzhen Gao,Jingyi Yang,Xiaotian Zhou,Zhongyi Liu,Meng Zhang
A series of CuCoAl catalysts derived from layered double hydroxides (LDHs) with adjustable Cu/Co ratios were prepared via a facile in situ structure topotactic transformation strategy. The comprehensive characterization results revealed that the introduction of Co element and the confined effect of LDHs jointly promoted the dispersion and stability of Cu species, as well as significantly increased the active specific surface area. Interestingly, Cu 1.5 Co 1.5 Al sample showed the superior performance for furfural (FF) hydrogenation to furfuryl alcohol (FA) under the synergistic effect of Cu 0 and Cu + species, as well as the interaction between Cu species and the support. It allowed for FF conversion of 97.5% and FA selectivity of 99.7% (150 °C, 3 h, 2 MPa initial H 2 pressure, isopropanol as solvent, m(FF):m(catalyst) = 60:1). Moreover, Cu 1.5 Co 1.5 Al displayed the satisfactory reusability, where the activity and selectivity kept stable after six successive recycling runs. Specially, it displayed the promising potential for the scale-up production. Furthermore, the mechanism study based on in situ Fourier transform infrared spectra indicated that the surface exposed Cu 0 species could promote the H 2 adsorption and then rapidly dissociated H 2 into the activated H atoms, whilst Cu + species were the active sites for FF selective hydrogenation in a η 1 (O)-aldehyde adsorption configuration.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
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IF 8.7
Ziwei Guo,Huan He,Kunqian Liu,Shicheng Yang,Zihui Li,Chaochao Lai,Zhicheng Liao,Xiaomin Ren,Bin Huang,Xuejun Pan
Insights into COVID-19 antivirals’ environmental fate and ecological risk are urgently required due to their increasing concentrations in aquatic environments, which have rarely been studied. Herein, we first investigated the photochemical transformation and the resulting alterations in toxicity of arbidol, an antiviral drug with relatively higher toxicity. The photolysis of arbidol was rapid with a rate constant of 0.106 min −1 due to its superior ultraviolet light absorption , in which the direct photolysis was predominated with a contribution of 91.5%. Despite its substantial photolysis, only 14.45% of arbidol was mineralized after 100 min, implying that arbidol and its products might have a long-term impact on aquatic environment. It was inferred that arbidol was photolyzed mainly via the loss of thiophenol, bromine, and alkylamine, based on twelve photolytic products identified. Notably, the experimental results demonstrated that the photolysis process increased the acute toxicity of arbidol, and the toxicity prediction indicated that the ecotoxicity of two photolytic products was very high with LC 50 values below 0.1 mg/L. Due to the co-effect of multiple constituents, the photolytic rate observed in wastewater treatment plant effluent and in river water was comparable to that in ultra-pure water, while it was slightly enhanced in lake water. The presence of dissolved organic matter suppressed arbidol photolysis, while NO 3 − exhibited a promotion effect. These results would be of great significance to assess the fate and risk of COVID-19 antivirals in natural aquatic environments.
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PubMed
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Bingyu Zhao,Haojie Li,Yuxiu Yu,Yaodong Liu
Carbon molecular sieve membranes (CMSMs) have exhibited significant potential in gas separation applications, particularly in the realm of hydrogen and carbon dioxide separation. Poly(furfuryl alcohol) (PFA) represents a cost-efficient and sustainable precursor utilized in the synthesis of CMSMs. Nonetheless, PFA-based CMSMs have exhibited suboptimal performance and frequently necessitate supplementary supporting layers. In the present investigation, we have explored various acids as catalysts for the in-situ self-polymerization of PFA. Our findings reveal that PFA membrane catalyzed by sulfuric acid exhibits the most favorable performance, yielding a hydrogen permeability of 1394.4 Barrer and a H 2 /CH 4 selectivity of 404.1. These values exceed the Robeson upper limits established in 2019. The enhanced gas separation performance of the sulfuric acid catalyzed PFA-based CMSM could be attributed to the increased furan ring opening and higher polymerization degree achieved through this catalytic process. Furthermore, our investigation delved into the addition of poly(styrene-co-acrylonitrile) (SAN) into the PFA membrane, yielding a CMSM featuring both dense and porous layers. With the addition of 6 wt% SAN in PFA membrane, the resulting CMSM exhibited a hydrogen permeability of 3126.4 Barrer, underscoring the potential for high-performance CMSMs made from the economical PFA precursor. The optimization of the PFA polymerization process and the incorporation of SAN, hold the promise of further elevating the performance of PFA-based CMSMs, and these advancements will substantially contribute to the advancement of sustainable and efficient gas separation technologies.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yuwei Li,Chengfeng Zhou,Xiaohan Zhang,Bin Hui
Developing high-performance and low-cost heterogeneous catalyst is an urgent need to activate peroxymonosulfate (PMS) towards organic pollutants degradation. Herein, a novel block catalyst comprising of iron oxide nanosheets and wood carbon (FeO X @WC) is proposed to enhance PMS activation for ciprofloxacin (CIP) degradation. The resultant FeO X @WC achieved the removal rate of 86.6% in 10 min. This hardwood-derived catalyst remained the excellent degradation performance in a wide pH range of 2.0–11.0 and the co-existence of other organic pollutants. Inspired by water circulation pathway in tree, a flowthrough degradation device was constructed via using the hardwood-derived carbon block with large vessel channels and small fiber tracheids channels in diameter. The removal rate reached 75.4% in 17 min for mass pollution solution (450 mL), suggesting the good degradation ability in practical application. Quenching experiments, electron paramagnetic resonance and electrochemical analysis reveal that non-radical pathways including singlet oxygen and electron transfer occupy the dominant effect. Nine intermediates were identified and three kinds of degradation pathways were proposed. This work provides a charcoal-based block catalyst to enhance the degradation efficiency towards aqueous CIP pollutants.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jian Zhang,Jia-Fang Xie,Jia-Cheng E. Yang,Ding Li,Lu-Bin Zhong,Yu-Ming Zheng
CoFe 2 O 4 /BHC-LDH3 catalyst was constructed by decoration of Co/Al layered double hydroxides (Co/Al-LDH) on bamboo hydrochar (BHC) loaded with magnetic CoFe 2 O 4 to activate peroxymonosulfate (PMS) for ciprofloxacin (CIP) degradation. Taking advantage of structural modulation and synergistic effects between the multi-components, CoFe 2 O 4 /BHC-LDH3 demonstrated high efficient PMS activation and ultra-fast CIP removal (91.50 % within 10 min), compared with BHC (6.26 %), CoFe 2 O 4 (26.32 %), and Co/Al-LDH (40.10 %). Both free radical (SO 4 – ) and non-radical ( 1 O 2 ) were crucial during the degradation process, and a substantial decrease in aquatic toxicity of the intermediates was observed. Additionally, the stability of CoFe 2 O 4 /BHC-LDH3 in actual water environment was tested using a fixed-bed reactor, illustrating the CoFe 2 O 4 /BHC-LDH3 has good stability and anti-interference ability in long-term operation. Possible degradation pathways of CIP in the CoFe 2 O 4 /BHC-LDH3 + PMS system were proposed based on liquid chromatography-mass spectrometer analysis and density functional theory calculation. This work provides new strategies for hydrochar-supported catalyst synthesis for organic pollutants decomposition.
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DIAMOND AND RELATED MATERIALS
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2023
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IF 4.1
Shuchang Wu,Min Zhao,Zhijun Xia,Junhui Liu,Yiquan Chen,Xiangxing Lv,Zhijian Jia,Zailai Xie
Tetracycline (TC) plays an essential role in both medical treatment and animal husbandry, but its abuse and accumulation in aquatic environments undoubtedly threatens ecosystems and human health. The advanced oxidation processes (AOPs) based on the activation of peroxymonosulfate (PMS) for the degradation of TC and other organic contaminants has attracted increasing attentions. Although metal-organic framework (MOF) derived transition metal‑nitrogen‑carbon material (MNC) shows fascinating potential for PMS activation, the direct carbonization of MOF makes limited active sites available for reaction due to serious agglomeration of the metal species together with the low yield of MNC catalyst. Herein, MOF composite (ZIF-67/NG) is designed via the in-situ growth of ZIF-67 on the N-doped graphene-like carbon (NG). The obtained Co@NC/NG after pyrolysis of ZIF-67/NG enabled the exposure of more active sites without notable aggregation of the Co nanoparticles . Co@NC/NG could effectively degrade TC via the activation of PMS and showed relatively good stability. Meanwhile, it was also highly active in wide pH range and the coexistence of inorganic anions as well as humic acid. Compared to bare ZIF-67 derived Co@NC, Co@NC/NG exhibited higher TOF value. The quenching experiments combined with EPR analysis indicated that both radical and non-radical routes were involved during the TC removal. Superoxide radicals, singlet oxygen and the surface bounded reactive oxygen species were important to the reaction. In comparison, sulfate radicals only made slight contribution and the effect of hydroxyl radicals could be omitted.
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CATALYSIS COMMUNICATIONS
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2023
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IF 3.7
Linsong Yang,Yuting Liu,Yu Peng,Yu-Cai He,Cuiluan Ma
The feasibility of chemobiocatalytic production of furfuryl alcohol from biomass-derived D -xylose was investigated using a tandem catalysis with deep eutectic solvent betaine:benzenesulfonic acid (DES BE:BA) and recombinant Escherichia coli DCF cell. The DES BE:BA (2.5 wt%) was applied to catalyze D -xylose under 170 °C for 0.5 h, resulting in a furfural yield of 51.1%. Consequently, recombinant Escherichia coli DCF fully transformed D -xylose-derived furfural to furfuryl alcohol in DES BE:BA-water under pH 7.5 and 40 °C using HCOONa as cosubstrate. This eco-friendly chemobiocatalytic strategy was successfully applied for transforming D -xylose to furfuryl alcohol in DES BE:BA-water.
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