Frontiers in Chemistry
·
2022
·
IF 5.545
Huo Zhaohui,Liao Yanmin,He Yongyi,Zhang Yifan,Liao Xiaolin,Zhang Qitong,Wu Haojie,Shi Junjie,Wen Genglong,Su Haixia,Yao Suyang
Graphitic carbon nitride (g-C3N4) has shown to be a promising photocatalyst that, however, suffers from strong charge recombination and poor conductivity, while MXenes have shown to be perfect cocatalysts for the photocatalytic process but show poor stability. In this study, we successfully constructed 2D/2D heterojunctions of Fe-C3N4/Ti3C2 for the photocatalytic degradation of antibiotics. In this study, multilayer Ti3C2 was obtained by etching Ti3AlC2, and then Fe-C3N4/Ti3C2 photocatalyst was prepared by the one-pot microwave method and high-temperature calcination method. The synthesized samples were characterized by XRD, SEM, TEM, XPS, TGA, BET, DRS, PL, and other means. The photocatalytic degradation of tetracycline hydrochloride by Fe-C3N4/Ti3C2 was in accordance with the first-order reaction kinetics model, and the apparent rate constant k was 2.83, 2.06, and 1.77 times that of g-C3N4, Fe-C3N4, and g-C3N4/Ti3C2, respectively. Through the mechanism study, it was shown that the most active species in the reaction system was • O2−, while h+ and •OH had a relatively lower effect on the degradation system.
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高影响因子
Chemical Engineering Journal Advances
·
2023
·
IF 0
Mengsi Cheng,Ying Fang,Zhaoguang Yang,Xinghao Liu,Bo Qiu,Tong Zhang,Haipu Li,Wenbo Zhao
MIL-100(Fe) was modified by amino groups (MIL - 100(Fe) - NH 2 ) to enhance the removal of antimonate (Sb(V)) with low concentration (50−200 μg/L) from natural water through batch adsorption experiments. With the initial Sb(V) concentration up to 200 μg/L, the residual Sb(V) concentration after treated by MIL - 100(Fe) - NH 2 was only 3.52 ± 0.131 μg/L, lower than the drinking water standards (5 μg/L) in China, while that was much higher (94.2 ± 3.52 μg/L) after pristine MIL-100(Fe) treatment. Based on results of XPS analysis, and adsorption kinetics and isotherms, we concluded that Sb(V) substituted the terminal −OH groups of MIL-100(Fe) to form inner-sphere complexes by coordination reactions with Fe nodes and be adsorbed by hydrogen bonding as well. The grafted amino groups (−NH 2 ) adsorbed Sb(V) by hydrogen bonding and facilitated the coordination reactions between Sb(V) and Fe nodes. The higher K L value (0.0116 ± 0.00,118 L/μg) obtained by fitting with the Langmuir isotherm model, while that of unmodified MIL-100(Fe) was 4.74 × 10 −4 ± 5.85 × 10 −5 L/μg, also confirmed that the −NH 2 groups greatly enhanced the affinity between MIL-100(Fe) and Sb(V). Furthermore, MIL - 100(Fe) - NH 2 still worked nicely in a wide pH range (2 − 12), with varied ionic strength (0.05 µmol/ L −1.5 mol/L), coexisting ions (CO 3 2− , NO 3 − , SO 4 2− , Cl − , H 2 PO 4 − ), and even in the real water bodies. Additionally, MIL - 100(Fe) - NH 2 exhibited good reusability and low Fe leaching (99.92 μg/L). We hope MIL - 100(Fe) - NH 2 become a candidate for effective removal of Sb(V), even other heavy metals from natural waterbodies.
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ACS Omega
·
2021
·
IF 3.512
Qirui Guo,Chong Chen,Fangcheng Xing,Weizhong Shi,Jie Meng,Hui Wan,Guofeng Guan
Nitrogen-doped hierarchical porous carbons with a rich pore structure were prepared via direct carbonization of the poly(ionic liquid) (PIL)/potassium ferricyanide compound. Thereinto, the bisvinylimidazolium-based PIL was a desirable carbon source, and potassium ferricyanide as a multifunctional Fe-based template, could not only serve as the pore-forming agent, including metallic components (Fe and Fe3C), potassium ions (etching carbon framework during carbonization), and gas generated during the pyrolysis process, but also introduce the N atoms to porous carbons, which were in favor of CO2 capture. Moreover, the hierarchically porous carbon NDPC-1-800 (NDPC, nitrogen-doped porous carbon) had taken advantage of the highest specific surface area, exhibiting an excellent CO2 adsorption capacity and selectivity compared with NDC-800 (NDC, nitrogen-doped carbon) directly carbonized from the pure PIL. Furthermore, its hierarchical porous architectures played an important part in the process of CO2 capture, which was described briefly as follows: the synergistic effect of mesopores and micropores could accelerate the CO2 molecules’ transportation and storage. Meanwhile, the appropriate microporous size distribution of NDPC-1-800 was conducive to enhancing CO2/N2 selectivity. This study was intended to open up a new pathway for designing N-doped porous carbons combining both PILs and the multifunctional Fe-based template potassium ferricyanide with wonderful gas adsorption and separation performance.
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高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Yuelong Xu,Ran Wang,Jingyue Wang,Yaru Zhang,Tifeng Jiao
Hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) serve as the most promising electrochemical processes for renewable energy. Developing multifunctional electrocatalysts with high performance for HER, OER and ORR still remains a challenge. Herein, we report a facile method to prepare P, N-co-doped porous carbon encapsulated Fe-CoP (A-Fe-CoP/CPN) electrocatalyst through freeze drying, carbonization, and KOH activation. The acquired A-Fe-CoP/CPN possesses abundant pores with large surface area, which provides sufficient defect-rich sites for HER, OER, and ORR, in alkaline or acidic electrolytes. The A-Fe-CoP/CPN shows low overpotential and good stability for HER and OER in alkaline electrolyte. Density functional theory (DFT) computations reveal that the addition of Fe greatly facilitates the rate-determining step and overall catalytic pathway for both HER and OER. A-Fe-CoP/CPN also exhibits low half-wave potential ( E 1/2 ) for ORR, which indicates an enhanced performance than that of the noble Pt/C catalyst. Zn-air battery equipped with the A-Fe-CoP/CPN catalyst exhibits a high energy density (849 mAh g −1 ) and a long-time stability at 5 mA cm −2 . This finding not only offers a facile strategy to prepare porous carbon materials with defect-rich sites, but also provides guidance for developing multifunctional electrocatalysts for wide electrochemical reactions.
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高影响因子
WATER ENVIRONMENT RESEARCH
·
2020
·Vol. 92
·期 8
·1142-1151
·
IF 1.369
Jingyao Huang,Muhammad Danish,Xihao Jiang,Ping Tang,Qian Sui,Zhaofu Qiu,Shuguang Lyu
The performance of trichloroethylene (TCE) degradation by sodium percarbonate (SPC) activated with Fe(II) in the presence of 3.0 g/L sodium dodecyl sulfate (SDS) as well as the role of SDS in the SPC/Fe(II) system was investigated since SDS is a common surfactant used in groundwater remediation for improving TCE dissolution to the aqueous phase. The results showed that though the introduction of SDS could inhibit the TCE degradation, the inhibiting effect was less with the increasing SDS dose. In the presence of SDS, TCE could be completely removed with the SPC/Fe(II)/TCE molar ratio of 40/80/1. Experiments with free radical probe compounds and radical scavengers elucidated that TCE was mainly oxidized by both HO· and . A weakly acidic environment was more favorable to TCE degradation. Nevertheless, at a high concentration had a strongly inhibitive effect on the TCE degradation but the influence of Cl − was negligible. Finally, the excellent TCE degradation achieved in actual groundwater demonstrated that Fe(II) activated SPC technique was applicable in the remediation of TCE contaminated groundwater in the presence of SDS. Practitioner points The effects of SDS were evaluated SPC/Fe(II)/SDS system applied to remediate TCE The mechanism of HO· and generation had been investigated Cl − and affected TCE degradation at different levels The performance of TCE removal in actual groundwater had been studied
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高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2023
·Vol. 149
·期 9
·04023052
·
IF 2.2
Xincheng Ye,Jie Yao,Zekun Dong,Yan Zhang
The novel Fe-doped MoS2/granulated activated carbon (GAC) particle electrodes (FMG PEs) were controllably synthesized by a hydrothermal method and used in the three-dimensional (3D) electroactivation of peroxydisulfate (E-PDS-FMG) for carbamazepine (CBZ) degradation. The performance, mechanism, and influencing factors of CBZ degradation by the E-PDS-FMG system were systematically discussed. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) analyses showed that the E-PDS-FMG system has an excellent conductivity and a high electron transfer rate and exhibited a superior electrocatalytic performance for CBZ degradation. A CBZ removal rate greater than 99% can be achieved within 25 min under the conditions of FMG dosage of 0.4 g L−1, PDS concentration of 2.0 mM, current density of 1.0 mA cm−2, and initial pH value of 5. Sulfate radicals (SO4·−) and hydroxyl radicals (OH) were recognized as the major active species through quenching experiments and electron paramagnetic resonance (EPR) measurement. In addition, Fe (IV) was also involved in the E-PDS-FMG system according to the transformation of methyl phenyl sulfoxide (PMSO) to methyl phenyl sulfone (PMSO2). Furthermore, the possible mechanism of the E-PDS-FMG system was proposed. FMG PEs were applied as the catalyst and particle electrodes for PDS activation, improving the yield of OH, SO4·−, and Fe (IV). The increase of FMG dosage and PDS concentration accelerated the degradation of CBZ, and the E-PDS-FMG system exhibited a high degradation ability on CBZ removal in a wide pH range. The results all indicate that the E-PDS-FMG system is a promising technology for organic pollutant removal from water due to its excellent electrocatalytic performance and remarkable stability.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Baicheng Yuan,Xinyi Huang,Shaojinlin Yang,Yi Yang,Zhihong Lin,Raphael Semiat,J. Paul Chen
Heavy metal contamination has become one of the greatest global environmental problems. In this study, a magnetic calcium-alginate hydrogel-sphere encapsulated with Fe–Mn–Zr ternary-metal composite (MCHETC) was prepared through a combined co-precipitation and extrusion approach and used for the adsorption of heavy metals in aqueous solutions. The active sites were dispersed in the MCHETC, which can be separated by the magnetic force for the ease in operation. Above 80% of ultimate adsorption was completed at a contact time of 5 h. The copper uptake history was well described by the intraparticle surface diffusion model, suggesting a multi-step process for the adsorption. The optimum pH for adsorption was 4; the maximum adsorption capacity was 103.1 mg-Cu/g. The adsorption capability well remained after the 5 adsorption–desorption cycles and the copper could be recovered. Furthermore, the adsorbent performed well in the nature water spiked with copper ions. The mechanism studies illustrated that the adsorption was mainly controlled by the ion-exchange reaction. This study demonstrated that the MCHETC adsorption technology may be used for heavy metal removal and recovery with higher efficacy.
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高影响因子
ChemNanoMat
·
2022
·Vol. 8
·期 6
·e202200085
·
IF 3.82
Yang Gu,Chuqian Meng,Shuyue Dong,Hexin Zhu,Qian Liu,Yonglan Luo,Qingquan Kong,Tingshuai Li
High-performance earth-abundant electrocatalysts for oxygen evolution reaction (OER) are highly desirable. In this report, we successfully synthesized amorphous Fe−P shell electrodeposited on Co(OH)F nanowire arrays supported on titanium mesh (Fe−P@Co(OH)F/TM) as an efficient catalyst for OER. Such catalyst exhibits excellent OER activity with a low overpotential of 267 mV to reach the geometrical current density of 10 mA cm −2 in 1.0 M KOH. In addition, it has good electrochemical durability to maintain its activity for at least 20 h.
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高影响因子
WASTE MANAGEMENT & RESEARCH
·
2024
·
IF 3.7
Yan Zhou,Wenhui Liu,Dandan Chen,Bangwei Liu,Ping Lu,Yiwei Zhang
A novel Fe/Ca-modified biochar (BC) derived from corn stalk was prepared in this study for the simultaneous adsorption and immobilization of arsenic, cadmium and lead in aqueous solution and soil, respectively. The adsorption experiment in aqueous solution indicated that 1Ca-Fe@BC exhibited excellent removal efficiency (R, %) towards arsenic (46.3%), cadmium (76.3%) and lead (93.6%). The presence of cadmium and lead could enhance the adsorption efficiency of arsenic by facilitating the formation of ternary complexes with it. Moreover, both cooperative and competitive effects occurred between cadmium and lead adsorption. When the distribution coefficient of cadmium and lead was equimolar, cooperative adsorption prevailed. However, when the distribution coefficient deviated from this balance, competitive adsorption dominated with a higher affinity for lead. The soil culture experiment demonstrated that the utilization of 1Ca-Fe@BC could enhance the stability of arsenic, cadmium and lead in soil by enhancing soil cation exchange capacity and pH while reducing dissolved organic carbon. The competitive and cooperative effects of arsenic, cadmium and lead in soil were consistent with those found in aqueous solution. The results showed that 1Ca-Fe@BC exhibited an excellent remediation efficiency for both arsenic, cadmium and lead-contaminated aqueous solution and soil.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Chi Wei,Gaoxu Huang,Jiayi Mao,Jia Cai,Xiaopan Jin,Mengjia Guan,Feng Yu,Bin Dai,Yongsheng Li
Sodium metal batteries (SMBs) are attracting intensive attention as an appealing candidate for high-energy-density batteries, owing to the high specific capacity, rich abundance, and low cost of metallic sodium (Na). However, the practical application of SMBs has been greatly hindered by the uncontrollable dendrite growth and unstable solid electrolyte interfaces, which are responsible for the poor Na stripping/plating reversibility and short lifespan. Herein, we report an atomically dispersed Fe-doped mesoporous carbon nanosphere (Fe-MCN) as a sodiophilic host for facilitating homogeneous Na nucleation and deposition behaviors. Benefitting from the advantages of uniform mesoporous structures with large surface areas and atomically dispersed Fe doped in the carbon nanospheres, low nucleation barriers and subsequent homogeneous deposition behavior of Na metal are achieved, which give rise to highly reversible stripping/plating performance and outstanding cycling stability. As a result, the Na||Cu cell based on Fe-MCN-modified Cu substrates exhibits outstanding electrochemical performance with a high Coulombic efficiency of 99.97% over 850 cycles, and an ultralong cycling lifespan of 2600 h at 1 mA cm–2 and 1 mA h cm–2 is demonstrated by the symmetric cell with Na@Fe-MCN@Cu anodes. Moreover, the Na3V2(PO4)3 full cell based on the Na@Fe-MCN@Cu anode guarantees outstanding cycling stability for 2000 cycles with a capacity retention as high as 84%, showing high potential in the practical application of SMBs.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Tong-hui Yang,Song Yue,Wei-wei Gong,Ren-qing Wang,Wei-da Hu,Xiao-pan Liu,Peng-zhao Gao,Hang Qin,Wen-ming Guo,Han-ning Xiao
Electrochemical nitrogen reduction reaction(eNRR) is a promising strategy for ammonia production because of its mild reaction conditions, high theoretical conversion rate, and green pollution. However, the strong stability of N N triple bond and competitive hydrogen evolution reaction (HER) limit the Faraday efficiency and ammonia conversion of eNRR. In recent years, the structural design of catalysts combined with external field enhancement to enhance the AC magnetic field electrocatalytic reaction has received extensive attention. In this study, an eNRR catalyst ( x Fe-M-TiO 2 ) with a high concentration of oxygen vacancies was constructed by the defect engineering strategy. The ammonia conversion rate of eNRR of 1.5Fe-M-TiO 2 was 7.35 μg h −1 mg cat −1 , and the Faraday efficiency was 22.69 %, which was 2 % higher than that before doping. The spin–orbit coupling effect induced by the AC magnetic field further improved the eNRR activity, in which the Faraday efficiency increased to 52.14 % (increased by 150 %), and the ammonia yield increased to 13.37 μg h −1 mg cat −1 (increased by 5 %). After 80 h of eNRR, the current density of the catalyst became 95 % of the initial current density, and the stability was good. Density functional theory calculation showed that Fe doping did not change the reaction mechanism of eNRR but increased the concentration of oxygen vacancy, resulting in a 0.62 eV decrease in the energy barrier of the first hydrogenation of eNRR, which was conducive to the occurrence of eNRR.
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高影响因子
Materials Chemistry Frontiers
·
2017
·Vol. 1
·期 10
·2065-2077
·
IF 0
Fu Yang,Bangbang Wang,Hang Su,Shijian Zhou,Yan Kong
Surface defective or heterojunction sites of catalysts generally afford remarkable catalytic activity thanks to their high-surface-energy. Regularly-generating multiple defective sites on the surface of a catalyst is exceedingly promising in many reactions. In this study, we report an unexpected Co/Fe–Co planar hybrid composite nanosheet with serried surface defects including surface biphasic junction sites or defective holes. A facile thermal-induced process was applied to trigger the generation of defective sites on planar Co/Fe–Co hydroxides. Through a controlled thermal process, massive serried CoO nanocrystals were in situ dissolved out of the surface of cobalt hydroxide, while defective surface holes were formed on the Fe-doped Co(OH)2 nanosheets under a prolonged thermal procedure. The morphology and microscale structure of the resulting Co/Fe–Co hybrid 2-dimensional (2D) composites were systematically examined by virtue of various characterization techniques. As expected, the obtained surface defective Co/Fe–Co planar composites showed obviously enhanced catalytic activity in the Fenton-like reaction. Based on a catalytic study, we proved that the CoO nanocrystals densely-distributed on thinlayer Co(OH)2. Uniformly-introduced Fe heteroatoms in the inter-structure of Co(OH)2, along with the formed surface defective holes on Fe–Co hybrid composites, are synergistically responsible for increased catalytic removal efficiency of MB in the presence of peroxomonosulfate.
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