CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jieru Guo,Ge Song,Minghua Zhou
Iron-based catalysts usually have a narrow pH application range and are easy to agglomerate and inactivate in the heterogeneous electro-Fenton (Hetero-EF) process. In this work, FeN-carbon nanotubes (FeN-CNTs) catalysts with highly dispersed FeNx sites and tubular structures were synthesized. This FeN-CNTs/Hetero-EF process extended the pH application range to 3–11 with low metal leaching (0.4 mg/L at pH 3) and negligible homogeneous contribution. Compared with nitrogen-doped carbon (N-C, prepared with the same procedure but without FeCl 3 ⋅6H 2 O precursor), its pseudo-first order reaction rate constant was increased by 4.4 times, suggesting that the uniformly dispersed active site FeNx played a key role in the catalytic activation of H 2 O 2 and the efficient degradation of carbamazepine (CBZ). Effective CBZ removal (10 mg/L) could be achieved at low current density (1.25 mA/cm 2 ) and catalyst dosage (50 mg/L) in FeN-CNTs/Hetero-EF. The capture experiments and EPR tests confirmed the existence of various active species such as • OH and 1 O 2 , among which • OH played a dominant role in the degradation of CBZ. FeN-CNTs significantly improves the removal of pollutants under a wide pH range, showing broad application prospects.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Wanqing Zhang,Haixian Liu,Yuxuan Xiao,Jie Ying,Hongwei Liu
Oxygen evolution reaction (OER) has gained increasing attention among researchers due to its significance in energy conversion. However, the sluggish kinetics of the OER present notable challenges. In this work, we present an energy-efficient, cost-effective, widely applicable, and scaled-up biological preparation method to prepare OER catalytic materials with high activity and stability based on bacteria and inexpensive Ni-Fe foam under mild conditions. Anaerobic sulfate-reducing bacterium Desulfovibrio caledoniensis and aerobic Pseudomonas stutzeri are the typical microorganisms and the OER performance of their products is not clear. Electrochemical measurements show that the catalyst prepared via D. caledoniensis exhibits a low overpotential of only 247 mV to achieve 10 mA cm −2 and a low Tafel slope of 46 mV dec -1 , while the catalyst prepared via P. stutzeri has an overpotential and Tafel slope of 259 mV and 71 mV dec -1 , respectively. Therefore, these catalysts exhibit excellent catalytic activities. Furthermore, they have a good stability of more than 40 h at 10 mA cm −2 which is far superior to that of the majority of reported NiFe-based OER catalysts. This work shows new insights into the preparation and development of high-performance OER catalysts in mild conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chengyu Huangfu,Shuning Yu,Bo Tong,Anni Yang,Jiafei Lyu,Xianghai Guo
MIL-100(Fe) is a kind of metal–organic frameworks (MOFs) with robust water and chemical stability. The adsorption kinetics, isotherms, thermodynamics and regeneration of MIL-100(Fe) were investigated to illustrate the process of efficient lithium adsorption. The adsorption kinetics of MIL-100(Fe) followed Pseudo-second-order model, and the lithium adsorption equilibrium was reached rapidly in 2 h. Langmuir model fit best with the adsorption isotherms, indicating chemisorption of lithium ions on MIL-100(Fe) and possibly a monolayer adsorption process. By calculating thermodynamic parameters (Δ G θ , Δ H θ and Δ S θ ), the adsorption of lithium on MIL-100(Fe) can be illustrated by a spontaneous endothermic process. The adsorption mechanism involved electrostatic interaction, impact of crystal defect sites and coordinative interactions between metal active sites and lithium ions (Fe—F‧‧‧Li). MIL-100(Fe) was regenerated for four cycles, and there was only a slightly decrease in adsorption capacity and the morphology remained stable. Combined with extremely short equilibrium time and high stability, MIL-100(Fe) can be a promising adsorbent for lithium extraction.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 31
·10662-10671
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IF 4
Dan Wen,Yan Ma,Guomei Mu,Qiuping Huang,Xuefeng Luo,Dunmin Lin,Chenggang Xu,Fengyu Xie,Guangzhao Wang,Wenhan Guo
Improving the efficiency of the anodic oxygen evolution reaction (OER) is important to solve the global energy crisis and greenhouse gas emission problems. In this paper, a preparation method for a MIL-53(Fe)@ZIF-67(Co) composite electrode is proposed. The hierarchical structure formed by the combination of MIL-53(Fe) and ZIF-67(Co) provides a rich channel for the transport of electrons and mass in the OER process. XPS analysis and DFT calculations revealed that Fe electrons in MIL-53(Fe) were transferred to Co in ZIF-67(Co) through O, which confirmed the rapid charge transfer effect of this transport channel. The MIL-53(Fe)@ZIF-67(Co) electrode has significant OER performance. When the current density reaches 10 mA cm−2, the overpotential is only 193 mV. This study inaugurates a new way for the rational design of a multiphase interface and the construction of new MOF channel structures.
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ENVIRONMENTAL RESEARCH
·
2023
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IF 8.3
Chuanhui Geng,Qingguo Chen,Zhenzhen Li,Mei Liu,Zhi Chen,Hengcong Tao,Qiao Yang,Baikang Zhu,Lijuan Feng
In this study, we investigated the doping of Fe–N–C with ZnO (Fe–N–C@ZnO) to enhance its performance in the reduction of biological toxicity and degradation of enrofloxacin (ENR) in seawater. The steady-state/transient fluorescence analysis and free radical quenching test indicated an extremely low electron–hole recombination rate and the generation of reactive oxygen species in Fe–N–C@ZnO, leading to an improvement in the energy efficiency. We compared the ENR degradation efficiencies of Fe–N–C@ZnO and ZnO using both freshwater and seawater. In freshwater, Fe–N–C@ZnO exhibited a slightly higher degradation efficiency (95.00%) than ZnO (90.30%). However, the performance of Fe–N–C@ZnO was significantly improved in seawater compared to that of ZnO. The ENR degradation efficiency of Fe–N–C@ZnO (58.87%) in seawater was 68.39% higher than that of ZnO (34.96%). Furthermore, the reaction rate constant for ENR degradation by Fe–N–C@ZnO in seawater (7.31 × 10 −3 min −1 ) was more than twice that of ZnO (3.58 × 10 −3 min −1 ). Response surface analysis showed that the optimal reaction conditions were a pH of 7.42, a photocatalyst amount of 1.26 g L −1 , and an initial ENR concentration of 6.56 mg L −1 . Fe–N–C@ZnO prepared at a hydrothermal temperature of 128 °C and heating temperature of 300 °C exhibited the optimal performance for the photocatalytic degradation of ENR. Based on liquid chromatography–mass spectrometry analysis, the degradation processes of ENR were proposed as three pathways: two piperazine routes and one quinolone route.
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Hong Yu,Chen Wang,Xinhe Xiong,Bitao Dai,Yang Wang,Zhijie Feng,Hao luo,Jiangxiong Zhu,Guoqing Shen,Yun Deng,Xueqing Geng,Danfeng Wang,Lumei Wang
Acetamiprid (Ace), extensively employed in agricultural production as a substitute for organophosphorus pesticides, poses a potential threat to the environment and human health due to excessive residues. Hence, the development of reliable and convenient techniques to determine Ace levels in the environment holds significant importance. Among various assay methods, nanomaterial-based aptamer-based biosensors (aptasensors) have emerged as efficient and promising tools. In this study, we successfully developed a novel aptasensor for monitoring Ace in the environmental water, utilizing advanced nanomaterials known as Fe-N-C single-atom nanozymes (SAzymes). Fe-N-C SAzymes exhibited excellent catalytic activity, high stability, and complete atom utilization. A facile dual-confinement route was employed for the synthesis of Fe-N-C SAzymes, and their performance as oxidase-like nanozymes was investigated. The synthesized Fe-N-C SAzymes presented distinct oxidase-like activity and demonstrated the capability to interact with a chromogenic indicator-TMB, serving as the signal transduction element in our assay. Furthermore, we found that thiol-modified aptamers could effectively dampen the oxidase-like activity of Fe-N-C SAzymes.Therefore, we successfully developed a Fe-N-C SAzymes assisted detection method for Ace, which exhibited high sensitivity (LOD = 16.9 nM) and selectivity. Overall, this work provides new insights into the design of multifunctional Fe-N-C SAzymes for environmental and biological applications.
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Xinru Xu,Chenyang Shu,Rong Jin,Hongdian Chen,Chuanlan Xu,Yao Liu,Lingtao Sun,Chaozhong Guo,Haifeng Chen,Wenli Liao
Low-density active sites, low-mass transfer rate, and poor stability of carbon-based catalytic materials from the pyrolysis of conventional metal-nitrogen complexes can hamper the oxygen reduction reaction (ORR). Herein, a composite structure of nitrogen-doped carbon nanosheets grafted with carbon nanotubes are synthesized by Zn-ZIF-L breaking and co-functionalized by coupling Fe 2 O 3 nanoparticles with active Fe-N x species to form an active ORR catalyst (D-FeNC/MOF). Under the synergetic effect of high-density active sites and multi-size pore distribution, the diffusion resistance of oxygen in the pores can be decreased to facilitate the transfer of reactants and products, and the improvement of ORR efficiency. Comparing to the commercial Pt/C catalyst, the d -FeNC/MOF has exhibited a more positive half-wave potential of 0.875 V ( vs . RHE) and a higher catalytic stability. Besides, the zinc-air battery assembled with d -FeNC/MOF as a cathode catalyst can also offer a maximum power density of 170 mW cm −2 and a specific energy density of 842 Wh kg −1 . This work can provide a new way for designing non-Pt catalysts for various electrochemical energy devices.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2023
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IF 10.9
Xin Wen,Cui Li,Hui Liu,Guohua Fan,Yanan Tang,Chuncheng Hao,Lili Ma,Pingan Song
Recently great efforts have been focused on designing high-performance microwave absorbers using sustainable biomass resources, but there remains a lack of green and efficient fabrication methods. Herein, inspired by natural porous character of biomass waste, we demonstrated a green one-step route to convert waste coffee grounds into porous C/Fe hybrids, and further explored their potential applications for broadband and high-efficiency microwave absorption. In this design, the WCG-20–750 (incorporated 20 wt% Fe(C₅H₇O₂)₃ catalyst and carbonized at 750 °C) exhibited porous microstructure with the highest char yield of 55.45 wt%. Furthermore, the as-prepared C/Fe hybrids from WCG-20–750 displayed excellent microwave absorption performances. Typically, the minimum reflection loss (RL min ) reached to -52.86 dB and the widest effective absorption bandwidth (EAB) was 6.40 GHz at the thickness of 3.0 mm. This work provides an economically viable and environmentally friendly strategy to convert biomass wastes into value-added microwave absorbers, ultimately making contributions to the upcycling of renewable biomass resources and the fostering of sustainable environment.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 39
·91262-91275
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IF 5.8
Cheng Tangying,Li Jinjin,Ma Xiuwei,Yang Linjun,Zhou Lei,Wu Hao
Various materials have been developed to capture volatile organic compounds (VOCs) to mitigate air pollution. However, sorbent materials with excellent resistance to water are rare. Here, several Fe/N-doped activated carbons (ACs) have been prepared to capture VOCs in humid environments. The ACs were analyzed by various characterization techniques, such as BET, SEM, XPS, XRD, FTIR, and Raman. The results showed that Fe/N doping resulted in the specific surface area of the ACs increasing by 500 to 1000 m 2 g −1 , the average pore size increasing to approximately 2 nm, improved mesoporous structure, higher graphitization, lower hydrophilicity, and polarity. The VOCs adsorption performance of the ACs was evaluated by static and dynamic adsorption experiments. The uptake of toluene and ethyl acetate by ACs was enhanced to 224 mg g −1 and 135 mg g −1 , respectively. And ACs were able to maintain 70 to 80% VOCs adsorption capacity for VOCs at 80% relative humidity. Furthermore, the microscopic mechanisms were investigated by the grand canonical Monte Carlo method (GCMC). The highly graphitized structure and the N functional groups favored the VOC adsorption process and discouraged the adsorption of water vapor. This work affirmed the dominance of Fe/N-doped carbon, which will contribute to the evolution of water-resistant VOCs adsorbent materials. Graphical Abstract
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Nanoscale
·
2023
·
IF 6.7
miaomiao yuan,Rongjun Zhang,Shuxiang Xu,Lihao Guo,Luoyijun Xie,Yingying Liao,Yang Xu,Xuemei Fu
Photothermal therapy (PTT) is an emerging field, and the photothermal agents could convert visible or near-infrared (NIR) radiation into heat to kill tumor cells. However, the low photothermal conversion efficiency of photothermal agents and their limited antitumor activities delay the development of these agents into monotherapies for cancer. Herein, we have fabricated an ultrasmall polyvinylpyrrolidone (PVP)-Fe-Cu-Ni-S (PVP-NP) nano-agent via a simple hot injection method with an excellent photothermal conversion efficiency (~96%). Photothermal therapy with this nano-agent effectively inhibits tumor growth without apparent toxic side effects. Mechanistically, our results demonstrated that, after NIR irradiation, PVP-NPs can induce ROS/singlet oxygen generation, decrease mitochondrial membrane potential, and release extracellular Fe2+ and consume glutathione, triggering autophagy and ferroptosis of cancer cells. Moreover, PVP-NPs exhibit excellent contrast enhancement according to magnetic resonance imaging (MRI) analysis. In summary, PVP-NPs have a high photothermal conversion efficiency and can be applied for MRI-guided synergistic photothermal/photodynamic/chemo-dynamic cancer therapy, solving the bottleneck of existing phototherapeutic agents.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Zhimin He,Zhengjie Tan,Yu Pu,Qiyu Li,Wei Hong,Rong Li,Xinglong Gou
Ti 3 C 2 T x nanosheets arrays sandwiched with FeNi 2 S 4 nanoparticles are in-situ grown on Ni-Fe foam (FeNi 2 S 4 -Ti 3 C 2 T x @NFF) via a facile one-pot hydrothermal route. The as-prepared FeNi 2 S 4 -Ti 3 C 2 T x @NFF exhibits simultaneously excellent catalytic activity towards oxygen and hydrogen evolution reactions with low overpotentials (136 and 97 mV at 10 mA cm -2 , respectively) and superior stability. Moreover, a symmetrical electrolyzer utilizing FeNi 2 S 4 -Ti 3 C 2 T x @NFF as the anode and cathode only requires 1.51 V for overall water splitting to reach 10 mA cm -2 , and can continuously operate at 20 mA cm -2 for 100 h. The outstanding catalytic performance of the catalyst can be attributed to increased active sites in the well-dispersed FeNi 2 S 4 nanoparticles, enhanced electronic conductivity due to introduction of Ti 3 C 2 T x nanosheets, strong electronic coupling between Ti 3 C 2 T x and FeNi 2 S 4 , improved mass transfer through the hierarchically porous structures and robust self-supporting configuration.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Xiangyu Wang,Min Jiang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu,Jun Ma
Although Fe/Fe 2 O 3 has potential application compared with nanoscale zero-valent iron (nZVI), its smooth structure largely limits the catalytic performance. To address this challenge, we innovatively constructed highly efficient composite Fe/Fe 2 O 3 @UiO-66 via employing an urchin-like core-shell structure of Fe/Fe 2 O 3 onto UiO-66 through a facile ion exchange precipitation method without inert gas protection. The characterization results show the urchin-like core-shell configuration can extend the life span of Fe 0 and produce more active sites. Besides, the absorption spectrum is broadened by Fe 2 O 3 which has narrow band gap and the high-efficiency separation of photogenerated electron-hole pairs is obtained with the load of Fe/Fe 2 O 3 . Moreover, Two-parameter pseudo-first-order decay model fits well with the reduction and adsorption of composites in the dark reaction, and a plausible pathway for tetracycline (TC) degradation is also proposed. The findings of this research provide a promising method for promoting the catalytic properties of MOF-based materials and Fe/Fe 2 O 3 .
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