Polymers
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2022
·Vol. 14
·期 14
·2959
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IF 4.967
Jun Wang,Xiaocui Wen,Shaojun Jiang,Tao Chen
Inappropriate disposal of leaching residues from the lead-zinc tailings recovery process may result in environmental pollution. Its recycling and reuse remain a prevalent topic in environmental science and technology. It was roasted to prepare leaching residues-based materials (TLRS) in this work, and the TLRS were creatively used as the catalyst to active sodium persulfate (PS) to degrade organic pollutants. Degradation of tetracycline using the TLRS–PS system was evaluated, and the treating parameters were optimized. Roasting resulted in the exposure of active sites on TLRS surface, in which transition metals can donate electrons to PS to form SO4·−. SO4·−can further react with OH−to form ·OH. Formation of these radicals was confirmed by both quenching experiments and EPR analysis. Under optimized conditions, 85% of the TC can be degraded in 3.0 h, and ~50% of degraded TC was mineralized to CO2and H2O. The performance of TLRS barely changed after four reuses, suggesting the chemical stability of TLRS. The presence of dissolved substance in the water matrix could weaken the performance of the TLRS–PS system. A mechanism of TC degradation was proposed based on the experimental results and literature. These preliminary results provide us new insight on the reuse of lead-zinc flotation tailings.Keywords:leaching residues;tetracycline;persulfate activation;oxidative degradation;solid waste
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Yajie Guo,Xinyu Zhang,Dandan Zhang,Shunlin Li,Hui Wang,Yiyin Peng,Zhaoyong Bian
The present work demonstrates a simple one-step pyrolysis method for the synthesis of a catalytic sludge-based carbon (SBC) biochar containing Fe and Mn from dehydrated sludge with added KMnO 4 and Fe(II). The electrocatalytic degradation of triclosan (TCS) in water was evaluated using an Fe/Mn-SBC cathode to promote a heterogeneous Fenton-like reaction. The catalyst generated at 500 °C exhibited an abundant porous structure and a relatively high surface area, and produced an electrode with better conductivity and electron diffusion . The presence of metal oxides changed the surface structure defects of this biochar and enhanced its catalytic performance while increasing the electrochemically active surface area by 72.68 mF/cm 2 compared with plain SBC. TCS was degraded (91.3%) within 180 min by oxygen species generated in situ on an Fe/Mn-SBC cathode because the activation energy for oxygen reduction was lowered by 4.62 kJ/mol. The degradation of TCS followed pseudo first-order kinetics and was controlled by TCS diffusion and interfacial chemical reactions between adsorbed TCS and the electrode. Possible TCS degradation pathways were devised based on the main intermediates, and 1 O 2 was found to be more important than •OH radicals. Through toxicity test and prediction, the toxicity of degradation was gradually reduced. This study demonstrates a simple and ecofriendly method for the electrocatalytic degradation of organic pollutants.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mengjie Pu,Daqi Ye,Jinquan Wan,Bentuo Xu,Wei Sun,Wei Li
A novel peroxymonosulfate (PMS) catalyst, zinc-based metal–organic framework electrospinning (ES) nanofibers membrane (short for ZIF-65/PAN) was firstly fabricated and used for the degradation of aqueous ciprofloxacin (CIP). Physicochemical properties, catalytic performance, stability, reusability, and the regeneration of ZIF-65/PAN was observed and conducted. Influence of various parameters including ZIF-65 loading content, reaction temperature, initial pH, and competitive organic molecules on CIP degradation was investigated. Reactive active species and degradation intermediates that involved in ZIF-65/PAN/PMS/CIP process were identified. Corresponding reaction mechanisms were speculated. The results indicate that the easy-separation ZIF-65/PAN nanofibers exhibit high efficiency for PMS activation, 89.2 % of CIP was degraded within 60 min, with up to 87.5 % of PMS utilization efficiency. ZIF-65/PAN was renewable through simple layer-by-layer self-assembly, thus shows good prospect in future applications. 26.4 % of surface Zn 2+ of ZIF-65/PAN exists in the form of + III oxidation state after activation, indicating the role of zinc catalytic site. Through activation, oxidative active species SO 4 ·− , ·OH, and 1 O 2 was generated, CIP was thus degraded through mainly-three pathways. This study provides novel ideas for the application of MOF-based membrane on PMS based advanced oxidation processes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yujie Cao,Tianran Sheng,Jinfei Mei,Peng Qian,Deqian Huang,Liangquan Sheng,Guoping Sheng
Herein, peroxymonosulfate (PMS)-like Fenton oxidation catalyst (DR-Vo-Co 3 O 4 ) with rich oxygen vacancies and carved flower-like structures were constructed using Co 3 O 4 as precursor via deep reduction strategy. DR-Vo-Co 3 O 4 could activate PMS to achieve almost 100% degradation of sulfadiazine (SD) within 1 min with ultra-high efficiency, possessing a degradation rate constant ( k ) value as high as 5.9 ± 0.2 min −1 , which was 86 and 5 times higher than the unreduced and reported maximum, respectively. Furthermore, the catalytic system showed unparalleled reactivity towards 14 different types of contaminants, with the maximum k value even exceeding 20 min −1 . The carved flower-like structure of DR-Vo-Co 3 O 4 catalysts not only facilitated PMS adsorption, but also provided more reaction sites for PMS activation. Meanwhile, rich oxygen vacancies could effectively tune the DR-Vo-Co 3 O 4 surface electronic state to further accelerate charge transfer, significantly enhancing PMS oxidation efficiency. Catalytic mechanism analysis revealed that 1 O 2 and O 2 •− played a dominant role in contaminant degradation.
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Catalysis Science & Technology
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2022
·Vol. 12
·期 19
·5879-5890
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IF 6.177
Dengfeng Dai,Chao Feng,Minmin Wang,Qingzhou Du,Dandan Liu,Yuan Pan,Yunqi Liu
Biomass-based chemicals as a renewable alternative to petroleum-based chemicals are of great significance. The conversion of biomass-based furfuryl alcohol to pentanediol, including 1,5-pentanediol and 1,2-pentanediol, is explored over a series of bifunctional Cu/MFI catalysts in a continuous-flow reactor. These catalysts are synthesized by supporting copper nanoparticles on MFI zeolites with varying molar ratios of SiO2/Al2O3. Among them, the Z60-10Cu catalyst containing balanced Cu0–Cu+ and Brønsted acid sites exhibits excellent performance, and a high furfuryl alcohol conversion of 99.5% and selectivity of 85.2% for 1,5-pentanediol (69.2%) and 1,2-pentanediol (16.0%) could be achieved (hydrogen pressure: 2.5 MPa) at 160 °C. The experimental results and the results obtained using the DFT technique revealed that the high catalytic activity realized during the processes of ring-opening and hydrogenation could be attributed to the synergistic effect between the Cu species and Brønsted acid sites. The Brønsted acid sites on the Si(OH)Al groups significantly affect the ring-opening process of furfuryl alcohol. The methoxy group on furfuryl alcohol adsorbs on the Cu+ sites, and the hydrogenation saturation of the ring-opening intermediate is realized under the influence of the activated hydrogen units on the Cu0 sites. The results reported herein could help promote the continuous production of high value-added pentanediol from biomass-based raw materials in the presence of non-noble metal catalysts. An economical and feasible path for the transformation of biomass resources into high value-added fine chemicals could also be developed.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Xiao Chen,Wenqi Liu,Jingjie Luo,Hongyu Niu,Rongrong Li,Changhai Liang
The hydrogenation of furfural containing multifunctional group often needs the high-efficiency cooperation of multiple catalytic active centers, which is greatly determined by the regulation of the surface and interface structure of multicomponent catalytic materials. Based on such circumstance, a series of highly dispersed supported bimetallic Cu–Ni catalysts prepared by the in situ topological transformation of layered double hydroxides have been investigated for the one-pot hydrogenation of furfural. Compared with the supported monometallic Cu and Ni catalysts, the optimized bimetallic Cu1Ni3/MgAlO catalyst presents highly efficient and good selectivity in the hydrogenation of furfural at the bath reactor. The selectivity to tetrahydrofurfuryl alcohol reaches 94.0% with a complete conversion of furfural at 110 °C under 3 MPa of H2 for 3 h. The results of TEM and in situ FT-IR confirm that the Ni-rich Cu–Ni alloy in the Cu1Ni3/MgAlO catalyst generates a strong synergistic effect, which shifts the adsorption configuration of furfural from parallel or vertical adsorption to tilted adsorption so as to significantly improve the catalytic performance. The intrinsic catalytic performances of CuxNiy/MgAlO catalysts indicate that the TOFC═O and TOFC═C values can be balanced through construction of the structure of the catalyst for achieving the synergistic effect between Cu and Ni significantly to enhance the one-pot selective hydrogenation of furfural to tetrahydrofurfuryl alcohol. Additionally, the Cu1Ni3/MgAlO catalyst presents excellent reusability by six-cycle testing. The above results indicate that the Cu1Ni3/MgAlO with the cooperation of multiple catalytic active centers is a promising catalyst for the selective hydrogenation of furfural.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yanping Sun,Jie Yu,Xiaohui Zhan,Lei Chen,Yue Zhao,He Wang,Huixiang Shi
In this study a copper-loaded N-doped carbon catalyst with mesoporous hollow sphere structure characteristic (Cu–NCHS) was prepared by in-situ synthesis followed with calcination and hydrothermal etching. Its catalytic performance for peroxymonosulfate (PMS) activation was evaluated using bisphenol A (BPA) as target pollutant. Owing to the coordination of more active sites provided by copper-loading and the mesoporous hollow structure characterized with high specific surface area (SSA) of 282.2 m 2 g −1 and large pore volume of 0.831 cm 3 g −1 , Cu–NCHS showed significantly better catalytic performance in BPA degradation (96.8% within 120 min) than those of NCHS (16.4%) and Cu-NC (19.6%) under the same initial conditions of BPA (20 mg L −1 ), PMS (100 mg L −1 ) and catalyst dosage (50 mg L −1 ). The possible mechanism of PMS activation by Cu–NCHS was also explored by ESR analysis and quenching experiments, and both radical and non-radical pathways were confirmed to be involved in BPA degradation process in Cu–NCHS/PMS system. Singlet oxygen ( 1 O 2 ), hydroxyl radical (•OH) and sulfate radical (SO 4 •− ) were identified to be the reactive oxygen species (ROS), of which 1 O 2 was the dominant ROS. Besides, the Cu–NCHS/PMS system showed excellent adaptability to pH change (from 3 to 11), common inorganic anions (Cl − , HCO 3 − , HPO 4 2− , SO 4 2− ) and natural organic matter (humic acid) in water. Meanwhile, the Cu–NCHS catalyst also showed good stability (with low Cu leaching of 0.14 mg L −1 ) and well reusability in recycling tests (the removal rate of BPA dropped by 14.0% after four successive runs). Combined with the experimental results in actual water (river water and wastewater), we demonstrated this study might provide a new insight for developing copper-loaded catalyst with high effect toward water treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Yuewen Shao,Kai Sun,Mengjiao Fan,Guoming Gao,Junzhe Wang,Lijun Zhang,Shu Zhang,Xun Hu
Copper-based catalysts are active for hydrogenation, while they are prone to sintering in hydrothermal conditions. In this study, alloying Cu with Ni and Zn was adopted to suppress sintering of copper species in the catalyzed conversion of furfural to cyclopentanone (CPO) and cyclopentanol (CPL) in the aqueous phase. The results indicated that Zn acted as a “glue” for aiding the formation of CuZn or CuNiZn alloy. The formation of the ternary CuNiZn alloy in CuNiZn/Al2O3 catalyst created the developed porous structure, induced the formation of abundant Lewis acidic sites and Brønsted acidic sites, and enhanced the dispersion and the total surface area of Cu species. These together rendered CuNiZn/Al2O3 with superior activity to monometallic or bimetallic Cu-based catalysts for the production of CPO and CPL (sum yield of 86% over Cu1.0Ni1.0Zn1.0/Al2O3), which was attributed to the synergy between CuNiZn alloy and Brønsted acidic sites. Alloying Ni with Cu and Zn weakened the adsorption of the C═C bond in the furan ring of furfural, while enhancing the activation of C═O and C–O–C bonds in furfural, avoiding the deep hydrogenation of the furan ring, facilitating the rearrangement of furfuryl alcohol to CPO, and improving the turnover frequency for the production of CPO from furfural remarkably (1011.3 h–1 over Cu1.0Ni1.0Zn1.0/Al2O3 vs 23.9 h–1 over Cu1.0/Al2O3). The formation of ternary CuNiZn alloy could not only suppress the sintering of metallic Cu species during the reduction in hydrogen but also effectively prevent the aggregation of Cu species in the aqueous phase, enhancing the catalytic stability under hydrothermal conditions.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Jiang Zhang,Zijian Wang,Mugeng Chen,Yifeng Zhu,Yongmei Liu,Heyong He,Yong Cao,Xinhe Bao
Deoxygenative upgrading of 5-hydromethylfurfural (HMF) into valuable chemicals has attracted intensive research interest in recent years, with product selectivity control remaining an important topic. Herein, TiO 2 supported gold catalysts coated with a thin N-doped porous carbon (NPC) layer were developed via a polydopamine-coating-carbonization strategy and utilized for pathway-specific conversion of HMF into 5-methylfurfural (5-MF) with the use of renewable formic acid (FA) as the deoxygenation reagent. The as-fabricated Au/TiO 2 @NPC exhibited excellent catalytic performance with a high yield of 5-MF (>95%). The catalytic behavior of Au@NPC-based catalysts was shown to be correlated with the suitable combination of highly dispersed Au nanoparticles and favorable interfacial interactions in the Au@NPC core-shell hetero-nanoarchitectures, thereby facilitating the preferential esterification of HMF with FA and suppressing unproductive FA dehydrogenation , which promoted the selective formylation/decarboxylation of hydroxy-methyl group in HMF in a pathway-specific manner. The present NPC/metal interfacial engineering strategy may provide a potential guide for the rational design of advanced catalysts for a wide variety of heterogeneous catalysis processes in terms of the conversion of biomass source.
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高影响因子
RENEWABLE ENERGY
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2022
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IF 8.634
Yuewen Shao,Jie Wu,Zhiyuan Zheng,Mengjiao Fan,Kai Sun,Félix Mérimé Bkangmo Kontchouo,Lijun Zhang,Shu Zhang,Guangzhi Hu,Xun Hu
Production of cyclopentanone (CPO) from biomass-derived furfural is attractive but challenging, as deep hydrogenation or ring-opening of furan ring in furfural over Co-based catalysts hinders the formation of the targeting products. In this study, alloying Co with Fe species in Co–Fe–Al catalysts is proposed for selective conversion of furfural to CPO in water. The formation of CoFe alloy in Co–Fe–Al catalyst weakened the interaction between Co species and the alumina carrier, lowered the adsorption/activation of H 2 , suppressed the formation of especially Brønsted acidic sites, facilitated the electron transfer from Co 0 to Fe species, increased the activation energy for hydrogenation of furfural (from 17.2 kJ mol −1 over Co–Al to 33.4 kJ mol −1 over 1.5Co-1.5Fe-1.0Al), and weakened the adsorption of C C and C–O–C functionalities in furan ring of furfuryl alcohol (FA) on metallic sites. These factors together suppressed deep hydrogenation of furan ring in FA or ring-opening of FA to diols, producing CPO and CPL with total yield of 91.5%, which was attributed to the synergy between hydrogenation and Brønsted acidic sites. In addition, the presence of Fe in Co–Fe–Al catalysts also enhanced the structural stability of Co species, preventing the phase transformation and aggregation of Co species, and rendering the catalyst with superior reusability .
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高影响因子
RENEWABLE ENERGY
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2022
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IF 8.634
Yunlong Yao,Zhiquan Yu,Chenyang Lu,Fanfei Sun,Yao Wang,Zhichao Sun,Yingya Liu,Anjie Wang
Copper catalysts showed excellent C O hydrogenation selectivity, but poor ability of hydrogen dissociation. Herein, a strategy to improve the activity of a Cu-based catalyst is developed by thermal treatment of Cu(OH) 2 at 100 °C with C 2 H 2 /Ar (0.5 vol%) followed by H 2 reduction at 300 °C. By means of X-ray diffraction (XRD), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS) and extended X-ray absorption fine structure (EXAFS), it was revealed that Cu x C crystallites , in addition to Cu crystallites, were present in the prepared catalysts. In furfural hydrogenation at 60 °C and 1.0 MPa, the Cu x C-containing catalyst showed significantly higher activity than the Cu counterpart prepared from the same precursor by H 2 reduction at 300 °C. The introduction of ZnO improved the dispersion, and thus led to enhanced catalytic performance. The Cu x C-Cu-ZnO catalyst with Zn/Cu molar ratio of 0.5 showed considerably high hydrothermal stability in a 70-h run, with furfural conversion of >99.0% and the furfuryl alcohol selectivity of 100%.
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