ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
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ACS Catalysis
·
2022
·
IF 13.7
Yuting He,Xiaoxuan Yang,Yunsong Li,Liting Liu,Shengwu Guo,Chengyong Shu,Feng Liu,Yongning Liu,Qiang Tan,Gang Wu
Single-metal site catalysts have exhibited highly efficient electrocatalytic properties due to their unique coordination environments and adjustable local structures for reactant adsorption and electron transfer. They have been widely studied for many electrochemical reactions, including oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). However, it remains a significant challenge to realize high-efficiency bifunctional catalysis (ORR/OER) with single-metal-type active sites. Herein, we report atomically dispersed Fe–Co dual metal sites (FeCo–NC) derived from Fe and Co co-doped zeolitic imidazolate frameworks (ZIF-8s), aiming to build up multiple active sites for bifunctional ORR/OER catalysts. The atomically dispersed FeCo–NC catalyst shows excellent bifunctional catalytic activity in alkaline media for the ORR (E1/2 = 0.877 V) and the OER (Ej=10 = 1.579 V). Moreover, its outstanding stability during the ORR and the OER is comparable to noble-metal catalysts (Pt/C and RuO2). The atomic dispersion state, coordination structure, and the charge density difference of the dual metal site FeCo–NC were characterized and determined using advanced physical characterization and density functional theory (DFT) calculations. The FeCo–N6 moieties are likely the main active sites simultaneously for the ORR and the OER with improved performance relative to the traditional single Fe and Co site catalysts. We further incorporated the FeCo–NC catalyst into an air electrode for fabricating rechargeable and flexible Zn–air batteries, generating a superior power density (372 mW cm–2) and long-cycle (over 190 h) stability. This work would provide a method to design and synthesize atomically dispersed multi-metal site catalysts for advanced electrocatalysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Minghui Xiang,Zhen Lu,Siyang Li,Hui Li,Chen Wang,Jin Zhang,Lide Jin,Chunyang Li
In recent years, new heterogeneous catalysts derived from metal organic frameworks (MOFs) have been widely used in advanced oxidation processes (AOPs). In this work, zeolite imidazole framework-67 (ZIF-67) and sulfide nanozero-valent iron (S-Fe) were used as precursors to prepare S-Fe/Co bimetallic nanoparticles embedded in graphitized carbon (S-Fe/Co@GC) and used to activate peroxymonosulfate (PMS) to degrade tetrabromobisphenol A (TBBPA). Morphological and structural characterization indicated that S-Fe/Co@GC compared to pre-carbonization, the pore size of the material became larger, formed a graphite carbon skeleton with excellent electrical conductivity. In a 0.2 g/L S-Fe/Co@GC and 0.6 mM PMS system, 96.1% of TBBPA (20 mg/L) was degraded within 30 min, and the degradation yielded a total organic carbon (TOC) removal of 56.2% in 60 min. This excellent catalytic activity was attributed to the synergistic effect of graphitic carbon, sulfide nanozero-valent iron and metallic cobalt. Radical quenching experiments and electron paramagnetic resonance (EPR) technology indicated that reactive oxygen species (ROS) included HO • , SO 4 •− , O 2 •− and 1 O 2 , among which O 2 •− plays a leading role in the degradation of TBBPA. Based on the LC-MS analysis of the degradation intermediates, the degradation pathway of TBBPA in the S-Fe/Co@GC/PMS system was proposed. In addition, S-Fe/Co@GC showed a low ion leaching rate, and the regenerated S-Fe/Co@GC still had high catalytic performance. This work will extend the development of MOFs encapsulate functional nanoparticle materials for environmental remediation.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
·
IF 10.319
Shuangqin Chen,Mai Li,Qingmin Ji,Tao Feng,Si Lan,KeFu Yao
Fe-based metallic glasses (Fe–MGs) are potential candidate catalysts for advanced oxidation processes (AOPs) for recalcitrant organic pollutant degradation. However, industrial wastewater and natural contaminated sites usually contain abundant inorganic ions, like the chloride ion (Cl − ), which significantly affect AOPs, but their influence on MG-activated AOPs still remains unclear. Through the study of three commonly used oxidants, hydrogen peroxide (H 2 O 2 ), peroxydisulfate (PDS), and peroxymonosulfate (PMS), the effect of Cl − on the FeSiB-catalyzed process of degradation of the typical azo dye Orange II was investigated. Evidence indicates that the addition of Cl − resulted in the monotonous inhibition of the degradation process when the H 2 O 2 /FeSiB and PDS/FeSiB systems were employed, but promoted effect was detected with the PMS/FeSiB system, which is different from the previously observed dual effect of Cl − . It is closely relative with FeSiB induced unique variety of degradation pathways, including radicals, non-radicals ( 1 O 2 ), and direct reduction degradation. Moreover, the presence of Cl − significantly affected the systems’ absorbable organic halogen content and the amount of Fe leached into the solution. The results of this work will provide essential references for Fe-based MG used as AOP catalysts in field applications and the development of advanced MGs with excellent adaptability to complex environments.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Chunxiao Zhang,Yingjie Li,Zirui He,Jianli Zhao,Dong Wang
Herein, a hollow microtubular Fe/Mn-promoted CaO-Ca 12 Al 14 O 33 bi-functional material was prepared by the bio-template method and used for H 2 production from sorption enhanced water gas shift (SEWGS). The microtubular Fe/Mn-promoted CaO-Ca 12 Al 14 O 33 exhibits excellent CO 2 capture and H 2 production performance in SEWGS/regeneration cycles. The stable hollow microtubular structure improves available adsorption and catalytic sites in Fe/Mn-promoted CaO-Ca 12 Al 14 O 33 for CO 2 capture and H 2 production. Mn addition improves CO 2 affinity capacity of the microtubular material. The Fe-Mn interaction increases redox ability of Fe 3+ /Fe 3+, 2+ , which promotes CO conversion. Moreover, the formed Ca 2 Fe 2 O 5 and Ca 2 MnO 4 both increase oxygen vacancies to promote catalytic activity of the microtubular material for WGS and its CO 2 capture capacity. The CO conversions for the microtubular material with the Fe/Mn/Al/Ca molar ratio= 10/2/10/100 are 98.7% and 94.0% after 20 cycles under the mild and severe calcination conditions, respectively. The hollow microtubular bi-functional material shows good prospect for efficient H 2 production from SEWGS.
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ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Yingjie Zhou,Feifan Wei,Haihua Wu
Electrocatalytic CO 2 reduction in solid oxide electrolysis cells (SOECs) can simultaneously convert CO 2 to valuable chemicals or fuels by integrating with renewable energy so as to alleviate the greenhouse effects and energy crisis. Cerium oxide (CeO 2 ) with high redox stability and catalytic activity toward CO 2 reduction is considered a promising SOEC cathode. However, CeO 2 is rarely directly employed as cathodes due to its unsatisfactory electrical properties. Suitable modification of CeO 2 becomes essential to improve its electrocatalytic activity . Herein, Fe-decorated on Sm-doped CeO 2 via a simple mechanical milling process was employed as cathodes for high-temperature CO 2 electrolysis in SOEC. The addition of Fe species on Sm-doped CeO 2 can greatly enhance the CO 2 electrolysis efficiency, mainly attributing to the increased catalytic active sites, electronic pairs, and oxygen vacancy concentrations, which facilitated the CO 2 adsorption and dissociation as well as the electron-ion transportation. The 1.0 wt.% Fe-decoreated on Sm-doped CeO 2 showed the highest current density of 0.57 A cm −2 at 1.9 V under 800 °C. Moreover, the co-existence of doped and surface coated Fe species on Sm-doped CeO 2 with moderate oxygen vacancies and adequate electronic transportation paths facilitate the high-temperature CO 2 electrolysis.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 17
·8271-8276
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IF 3.925
Ying-Xia Du,Lian Liu,Yong-Ke Li,Rui Liu,Wang-Ting Lu,Ji-Xiang Wang,Geng Zhang,Fei-Fei Cao
The preparation of two-dimensional (2D) composite material consisting of an active metal-based phase and carbon matrix is still a challenge. Herein, the 2D bimetal Co-TCPP(Fe) metal–organic framework (MOF) is synthesized and then adopted as the precursor to prepare a 2D composite electrocatalyst for the oxygen evolution reaction (OER). After carbonization and phosphorization, the 2D MOF is transformed into a composite nanoplate formed by Fe-doped CoP nanoparticles and a carbon matrix (Fe-CoP/C). This Fe-CoP/C composite exhibits a favorable OER performance in 1 M KOH with a low overpotential of 290 mV at 10 mA cm−2, which is better than that of counterparts without Fe and 2D morphology. The in situ formed metal (oxy)hydroxide is considered to be the main active species for the OER. The improved OER performance of Fe-CoP/C could be attributed to the Fe-doping in Co (oxy)hydroxide as well as the high electrochemical surface area induced by the 2D nanoplate morphology and conductive carbon network.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qiansheng Li,Hong Lu,Xiaolei Wang,Zhongqiang Hong,Ze Fu,Xinxin Liu,Jiti Zhou
Low solar energy utilization, instability of Fe ions and Fe(III)/Fe(II) cycle difficulty are three main factors, limiting the photocatalytic activity of the Fe/peroxymonosulfate (PMS) system. Herein, based on the N and Fe co-doped carbon dots (N, Fe-CDs) synthesized by a facile one-pot hydrothermal method, a new Fe(III)/Fe(II) cycle system for PMS activation under visible light irradiation was proposed. The characterization experiments showed that Fe has been successfully doped to the sp 2 graphitic structure and mainly existed as Fe-N and Fe-OH complexes, which played an important role in harvesting visible light, enhancing the stability of Fe ions and acting as active sites to accelerate electron transfer. Under visible light irradiation, the photogenerated electrons of N, Fe-CDs could be directly transferred to Fe (III) for Fe (II) formation via the ligand-to-mental charge transfer process, thus accelerating the Fe(III)/Fe(II) cycle. When N, Fe-CDs were used for activating PMS under visible light irradiation, aminopyrine could be efficiently degraded and mineralized to CO 2 via the cleavage of pyrazole ring, demethylation, hydroxylation, decarbonylation and the cleavage of benzene ring. The produced O 2 − and 1 O 2 played the main roles in the whole photocatalytic reaction. The above results revealed that the novel N, Fe-CDs could effectively activate PMS under visible light irradiation for the degradation of pharmaceuticals in the polluted water.
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JOURNAL OF MOLECULAR STRUCTURE
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2022
·
IF 3.841
Chenyan Wu,Qianhong Shen,Suhua Zheng,Xinyu Zhang,Jiansong Sheng,Hui Yang
A novel Bi 2 Sn 2 O 7 @MIL-100(Fe) composite photocatalyst was fabricated by loading Bi 2 Sn 2 O 7 nanoparticles on the surface of mesoporous MIL-100(Fe). The structure-property relationships of such composite photocatalyst were studied. The results exhibit that the formed Bi 2 Sn 2 O 7 @MIL-100(Fe) heterojunction promote the separation of photo-generated carriers, leading to the enrichment of photo-generated electrons on MIL-100(Fe). Meanwhile, MIL-100(Fe) can provide more active sites for photocatalytic reaction due to its extraordinary specific surface area. Therefore, the Bi 2 Sn 2 O 7 @MIL-100(Fe) composite photocatalyst exhibits excellent superoxide-radical-dominated photocatalytic activity and is more propitious to degrading the contaminants such as ciprofloxacin, which can be efficiently degraded in the absence of superoxide radicals. The Bi 2 Sn 2 O 7 @MIL-100(Fe) composite reveals enhanced photocatalytic activity for degrading ciprofloxacin with rate constant (0.0143 min −1 ) 1.96 and 3.86 times higher than that of pure MIL-100(Fe) (0.0073 min −1 ) and pure Bi 2 Sn 2 O 7 (0.0037 min −1 ), respectively.
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ANALYTICAL LETTERS
·
2022
·
IF 2.267
Yuhui Weng,Huangjie Li,Mincong Zhu,Aojia Tao,Sha Wang,Wen Weng
Novel nitrogen/iron-codoped carbon dots (N/Fe-CDs) were prepared from citric acid, ethylenediamine, and ferric chloride by a facile one-step solvothermal method and their peroxidase-like activity was evaluated. The structure and composition of the obtained carbon dots were characterized by several methods, including electron microscopy, X-ray diffraction, and spectral techniques. The presence of dopants in the particles was confirmed by X-ray photoelectron spectroscopy and inductively coupled plasma – mass spectrometry (ICP-MS). The obtained N/Fe-CDs displayed excellent peroxidase-like activity and efficiently catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine in the presence of H2O2, leading to a rapid change in the solution color from colorless to blue. Based on this reaction, H2O2 was determined from 0 to 40 μM under optimal conditions with a detection limit of 9.0 nM. In addition, L-cysteine was shown to cause the blue color to fade. Considering this feature, a highly sensitive, fast, and specific colorimetric method was developed for L-cysteine with a detection limit of 15.8 pM, which is lower than observed in similar studies. Further, this colorimetric method was applied for the determination of L-cysteine in real samples, and the results of recovery and relative standard deviation were satisfactory. The reported catalyst can be prepared conveniently using readily available raw materials and is inexpensive, which is advantageous for its widespread application.
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MOLECULES
·
2022
·Vol. 27
·期 6
·2035
·
IF 4.927
Jiao Jia,Hao Wu,Le Xu,Fengchun Dong,Yongtang Jia,Xi Liu
A nanofiber metal–organic framework filter, a polyacrylonitrile (PAN) nanofiber membrane composite with an iron/2-amino-terephthalic acid-based metal–organic framework (MIL101(Fe)-NH2), was prepared by one-step electrospinning. MIL101(Fe)-NH2was combined into the polymer nanofibers in situ. PAN-MIL101(Fe)-NH2composite nanofiber membranes (NFMs) were prepared from a homogeneous spinning stock containing MIL101(Fe)-NH2prebody fluid and PAN. Crystallization of MIL101(Fe)-NH2and solidification of the polymer occurred simultaneously during electrospinning. The PAN-MIL101(Fe)-NH2composite NFM showed that MIL101(Fe)-NH2was uniformly distributed throughout the nanofiber and was used to adsorb and separate acidic organic ionic dyes from the aqueous solution. The results of Fourier transform infrared spectroscopy, energy-dispersive X-ray spectroscopy, and X-ray diffraction analysis showed that MIL101(Fe)-NH2crystals were effectively bonded in the PAN nanofiber matrix, and the crystallinity of MIL101(Fe)-NH2crystals remained good, while the distribution was uniform. Owing to the synergistic effect of PAN and the MIL101(Fe)-NH2crystal, the PAN-MIL101(Fe)-NH2composite NFM showed a fast adsorption rate for acidic ionic dyes. This study provides a reference for the rapid separation and purification of organic ionic dyes from wastewater.Keywords:electrospinning;MIL101(Fe)-NH2;functional nanofibers;water treatment membrane
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JOURNAL OF RARE EARTHS
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2022
·
IF 4.632
Haining Song,Haifeng Zhou,Qianqian Zhuang,Zexin Li,Fenglei Sun,Zhenlei Yuan,Youxin Lou,Guangjun Zhou,Yujun Zhao
Oxidizing ClO − and IO 4 − exist widely in environment and are closely related to the health of organisms. Accordingly, fast, sensitive, and direct detection of the two species is significant. Using IFE in UCNPs @PAA and Fe(II)-phenanthroline system, an elegant ratiometric fluorescent nanosensor , without noble metal nanoparticle , was designed for the detection of ClO − and IO 4 − . Fe(II)-phenanthroline complex is used as fluorescent absorber, which can quench green light of UCNPs with gradually varied extent depending on the concentration of Fe(II). The linear zone extends to 800 and 120 μmol/L while the detection limit is 1.30 and 0.58 μmol/L for NaClO and NaIO 4 , respectively. Finally, the nanosensor was successfully applied to detect NaClO and NaIO 4 spiked in milk, spring water, and tap water with good recoveries.
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