Cell Reports Physical Science
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2022
·
IF 7.832
Xiao Wang,Lei Sun,Wei Zhou,Li Yang,Guoqing Ren,Hao Wu,Wei-Qiao Deng
The exploration of environmentally friendly and highly efficient oxygen evolution reaction (OER) catalysts is vital to large-scale, electrochemical renewable-fuels generation. Here, we report an iron single-atom catalyst (SAC) confined in a covalent organic framework (Fe-SAC@COF), which constitutes an unusual Fe–NO coordination in the skeleton. The as-prepared Fe-SAC@COF exhibits a high mass activity of 9.20 A mg −1 , which is 1.95 times higher than Ni species of the same coordination and 5.05 times higher than nanoparticulate Fe counterpart. Moreover, it shows, to the best of our knowledge, a record-low overpotential (290 mV) and Tafel slope (40 mV dec −1 ) among the reported atomically dispersed Fe-based catalysts and surpasses the benchmark Ir/C catalyst. The density functional theory calculation shows that the Fe–NO coordination exhibits low binding energy of oxygenated intermediates, which leads to an outstanding electrocatalytic OER performance. This work provides design strategies toward unusually coordinated SACs by prudent COF confinement for advanced electrocatalysis.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2015
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IF 2.711
Chongyi Li,Feng Xue,Enyong Ding,Xiaoling He
A unique organic–inorganic hybrid nanocomposite was designed and synthesized by chemically anchoring the cationic collagen-based derivatives onto the surface of Fe 3+ /TiO 2 nanospheres for the significant enhancement in photocatalytic activity under the visible light irradiation. The NMR analysis suggested the successful fabrication of cationic collagen-g-PDMC as grafted materials. In addition, the chemical structures, morphologies and properties of these samples were systematically characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), Raman spectrum, ultra violet–visible spectroscopy (UV–vis), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and photoluminescence (PL). And obtained results clearly demonstrated that Fe 3+ ions diffusing into TiO 2 lattice could be responsible for slightly reducing the average diameter of nanospheres to about 125 nm, promoting phase transition from anatase to rutile to some extent and extending the light harvesting range into visible region markedly. Meanwhile, the achievement that collagen-g-PDMC molecules had been covalently immobilized onto the surface of Fe 3+ /TiO 2 nanoparticles was also well supported by the information acquired. Furthermore, the photocatalytic activities of all the as-prepared products were carefully evaluated by adopting photocatalytic decoloration of methyl orange (MO) solution under the solar direct irradiation, and the sample CFT-3 performed the best in the photocatalytic degradation process, which was mainly attributed to the energetic synergistic effect brought about by Fe 3+ ions doping and collagen-g-PDMC molecules immobilized on the surface.
研究领域:
材料科学
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生物学
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环境科学
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高影响因子
Catalysts
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2022
·Vol. 12
·期 11
·1438
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IF 4.501
Guolei Liu,Xue Li,Qing Wang,Kuizhao Sun,Chuping Lee,Yue Cao,Weimeng Si,Haoran Wei,Zhongfang Li,Fagang Wang
In the work, a pig-blood-derived mesoporous carbon (BC) was prepared as a novel Fe-N-C material for the electrochemical sensor to detect hydrogen peroxide. Because of the unique nanostructure of Fe-BCs with rough surface structure, hierarchical pores, and high graphitization degree, the Fe-BCs, as a kind of advanced electrode material, exhibited remarkable performance in electrocatalysis. The sensor based on Fe-BCs exhibited an extra-long range from c and a detection limit of 0.046 μM (S/N= 3). The synthesis of low-cost, advanced carbon-based electrode materials from environmentally friendly pig blood for electrochemical sensor construction is a promising approach.
研究领域:
生物医学工程
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材料科学
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分析化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu
Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .
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DOI
PubMed
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 18
·7055-7074
·
IF 8.307
Rutong Song,Jun Yao,Mei Yang,Zhongbin Ye,Zhuang Xie,Xiang Zeng
Water pollution control is one of the major challenges currently faced. With the development of photocatalytic technology, an increasing number of new and efficient catalysts have been developed, but most of the catalysts have limited light capture ability and catalytic degradation efficiency. Therefore, in this work, hydrogen peroxide was further introduced to establish a photo-Fenton system to improve the photocatalytic effect by constructing a Z-scheme, and the degradation ability of the catalyst was maximized. Moreover, we successfully adhered bismuth tungstate nanosheets onto the surface of a MIL-101(Fe) framework and changed the number of active sites with iron ions of different doping amounts. We found that the number of active sites in the photo-Fenton system does not increase linearly, but increases and decreases regularly, which is similar to the change in band structure after doping. In addition, the results of the radical scavenger experiment and electron paramagnetic resonance (EPR) revealed that both hydroxide radical (˙OH) and superoxide radical (˙O2−) participated in methylene blue (MB) degradation, of which ˙OH was the main active species for pollutant degradation. Based on high-performance liquid chromatography-mass spectrometry (HPLC-MS) analysis, the possible degradation pathways were proposed. We believed that this work will provide insights into the heterojunction photo-Fenton system.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yanan Shang,Xinning Liu,Yanwei Li,Yue Gao,Baoyu Gao,Xing Xu,Qinyan Yue
The synthesis of a highly efficient and stable single atom catalyst (SAC) for peroxydisulfate (PDS) activation remains a challenge. Herein, a reconstructed iron single atom catalyst (Fe-SAC) with both abundant conjugated π-π sp 2 structured carbon and reactive Fe-N 4 sites was first reported to improve the decomposition of organics in PDS/SACs systems. Enhanced organics adsorption can be achieved by the conjugated π-π sp 2 structured carbon via π-π interaction to decrease the migration distance of reactive species to organic molecules. In addition, PDS tended to be attached onto the Fe-N 4 sites accompanied by the peroxymonosulfate (PMS) generation via S-O breakage of PDS, accelerating the generation of radicals. As a result, organics decomposition via PDS activation by reconstructed Fe-SAC was significantly higher (∼6 times) than the conventional Fe-SAC because of the synergistic effect of the resulting dual reaction sites. This work provides a new strategy to enhance the catalytic performances in PDS/SACs systems.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yizhuang Wang,Bingbing Liu,Hu Sun,Yanfang Huang,Guihong Han
Bauxite residue (red mud) is a typical solid waste discharged from the aluminum metallurgy industry and can be considered as an alternative resource for the recovery of iron (Fe), aluminum (Al), and titanium (Ti). Acid leaching is an effective technique for the simultaneous extraction of valuable metals from red mud, whereas the leachate with various metals confronts the difficulty of metals separation. In this work, a selective separation and recovery of Fe, Al and Ti from red mud leachate by the preferential Fe-Ti iso precipitate flotation followed by a reduction-hydrolyzation process was proposed. In the iso precipitate flotation process, the cupferron was acted as an Fe-Ti synchronous chelation agent and hexadecyl trimethyl ammonium bromide (CTAB) was used as an anionic collector for the flotation separation of Fe-Ti chelate. The generated fine hydrophobic chelates are rapidly separated from solution by flotation with the assistance of CTAB, in which 99.3% Fe and 99.8% Ti were transferred into the flotation product, while 96.7% Al remained in the leachate, realizing the first separation of Al. Reduction-hydrolyzation was further conducted to separate Ti and Fe from the dissolving solution of the flotation product. Hydrolysis thermodynamic analysis indicated that the required hydrolysis pH range of Fe 2+ was much different from that of TiO 2+ and Ti 3+ . After selective reduction of Fe 3+ to Fe 2+ by KI, 99.8% Ti was concentrated in the residue while 94.8% Fe remained in the solution. Eventually, the comprehensive recoveries of Fe, Ti, and Al are 94.1%, 99.7%, and 96.7%, respectively.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Runliang Zhu,Yanping Zhu,Haiyang Xian,Lixia Yan,Haoyang Fu,Gangqiang Zhu,Yunfei Xi,Jianxi Zhu,Hongping He
The generation of Fe(II) from Fe(III) is the rate-limiting step in the heterogeneous Fenton reaction, and accelerating this step is critical for enhancing the reaction efficiency and also the subject of extensive studies. In this work, the oxidized multi-walled carbon nanotubes (CNTs) were coupled with ferrihydrite (Fh) to synthesize novel and highly efficient heterogeneous Fenton catalysts (CNTs/Fh). Interestingly, the calculated apparent rate constants by 3%CNTs/Fh could reach ∼7.1 times as high as that by Fh, well in agreement with the accelerated decomposition rate of H 2 O 2 , as well as the enhanced generation rate of Fe(II) and hydroxyl radicals in the CNTs/Fh system. The density functional theory calculations and the cyclic voltammograms curves both well indicated that the Fe(III)/Fe(II) redox cycling on CNTs/Fh could be significantly enhanced during the Fenton reaction, from both dynamic (accelerating the electron transfer from H 2 O 2 to Fh) and thermodynamic (lowering Fe(III)/Fe(II) redox potential) aspects.
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高影响因子
FUEL
·
2024
·
IF 6.7
Guosheng Li,Yu Ding,Xiaohan Li,Kunhong Li,Xinrui Yin,Liang Zhao,Shenyong Ren,Chunming Xu,Baojian Shen
Regulation of electronic structure of metal active phase for catalysts has been known as efficient in promoting its catalytic activity; however, manipulating the activity of catalysts via controllable metal active phase electronic structure is still challenging. A non-equilibrium electronic structure Fe-based bulk catalyst has been developed via controllably adding P species, where the non-equilibrium electronic structure of Fe species is formed through the electron transfer from the Zn species through the P electronic channel. As a result, the catalytic activity of the modified Fe-based bulk catalysts has increased by 24.4–50.4%. Meanwhile, the sulfurization degree (SD) of the modified Fe-based bulk catalysts has increased by 5.6–25.9%. In addition, the HDS reaction rate constant ( k HDS ) has increased by about 2.0 times, and the DDS reaction rate constant ( k DDS ) has increased by about 2.4 times. The P modifying can regulate the directional transfer of unpaired free electrons between Fe and Zn species to form a more non-equilibrium electronic structure of Fe species, which can reduce the energy barrier of the C–S bond adsorbed on the P-modified Fe-based bulk catalysts. Importantly, the P species can be used as an active site to adsorb S-containing compounds in the modified Fe-based bulk catalysts, which is conducive to generating more coordinatively unsaturated sites (CUSs). The former can promote the formation of the more non-equilibrium electronic structure of Fe species, and the latter can adjust the adsorption active site of S-containing on the catalyst surface. Therefore, an electron transfer channel is formed among Fe, Zn, and P species, and another one is formed among Fe, P, and S-containing compounds, which form a dual-channel electron transfer behavior. Furthermore, the specific surface area, total pore volume, and reducibility of the modified Fe-based bulk catalysts have also shown varying degrees of improvement via the controllable addition of P species.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Mengkun Luan,Xiangjie Lei,Yu Fan
To increase the yield of light olefins during the catalytic pyrolysis of alkanes, a novel hierarchical Fe-incorporated ZSM-5 molecular sieve (FeM-Z5) was synthesized using an Fe-based metal-organic framework (Fe-MOF) as a mesoporogen and iron source through the dry gel conversion (DGC) method. In contrast to the conventional method of incorporating Fe species into ZSM-5 via impregnation, the DGC method incorporates Fe species into the framework of ZSM-5, decreasing the amount of Brønsted (B) acid sites and thereby inhibiting the side reactions of hydrogen transfer during the catalytic pyrolysis of alkanes. Compared with the FeN-Z5 catalyst prepared by the DGC method with Fe(NO 3 ) 3 as an iron source, FeM-Z5 had a larger amount of strong B acid sites and more mesopores with a size range of 10–40 nm originating from the decomposition of Fe-MOF; these aspects improved n-pentane pyrolysis and ethylene and propylene diffusion. As a result, the optimal FeM-Z5 catalyst exhibited the highest yield of ethylene and propylene (33.4 wt%) and the lowest deactivation rate (0.07 %/h) among the prepared catalysts during the catalytic pyrolysis of n-pentane.
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高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Shu Wang,Nanqi Ren,Danhui Liang,Jifei Chang,Xin Wang,Jiaguo Yan,Xiang Cheng,Lili Dong,Nan Li
Vivianite is an important bio-induced product of dissimilated iron reduction (DIR), which exists widely in activated sludge and digested sludge of wastewater treatment plants (WWTPs). Extracellular polymeric substances (EPS) surrounding dissimilatory iron-reducing bacteria (DIRB) were reported to be transient media for microbial extracellular electron transfer (EET) and DIR. However, what happens when a layer of EPS envelops microbial cells during vivianite recovery? This study tried to assess the relationship between iron reduction and electron transfer by stripping EPS layer-by-layer, then clarified the delamination of different EPS layers on the performance of vivianite recovery. After stripping total EPS (PC-EPS batches) of DIRB, the Fe (III) reduction efficiencies ( R Fe ), Fe (III) reduction rate ( V Fe ), and vivianite formation efficiency ( R V ) decreased by 33%, 37%, and 30%, respectively. Tightly bound-EPS (TB-EPS) was confirmed to play a crucial role in vivianite formation, which contributed 28–51% to vivianite recovery and 34–55% to iron reduction. Electronic shuttle substances were contained in TB-EPS, which enhanced the EET rate and efficiency between cells and Fe (III). The polysaccharide content of TB-EPS was positively related to adhesiveness between cells and mineral, as well as the iron reduction efficiency. Furthermore, redox proteins (PpcA, OmcB) were embedded in EPS, which shortened the distance of electron hopping to across the EPS layer and further accelerated vivianite recovery from wastewater. Long-term operation of anaerobic reactors confirmed that TB-EPS played critical roles in bio-induced vivianite formation.
研究领域:
环境科学
·
微生物学
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污水处理
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生物地球化学
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DOI
高影响因子
CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Jiaxing Ban,Barbara Lothenbach,John L. Provis,George Dan Miron,Zeyu Zhou,Dengquan Wang,Sergey V. Churakov,Bin Ma
Hydrotalcite-group layered double hydroxide (LDH) phases are important in many technical and geological contexts, and in applications ranging from environmental processes to catalysts to cements. This study systematically investigates the roles of Fe in LDH structures across varying pH conditions relevant to concrete environments, combining laboratory-based characterization, synchrotron-based techniques, and thermodynamic modeling. Elevated pH enhances Fe incorporation into the LDH phase, while suppressing ferrihydrite formation. At pH > 11, partial LDH dissolution is observed. Thermodynamic modeling and diffractometry reveal the transformation mechanism: control of the initial pH increases promotes Al(III) and Fe(III) uptake into LDH structures, while further alkalinization (pH > 11) triggers selective Al(III) dissolution, thereby increasing the M 2+ /M 3+ ratio and altering unit cell parameters. These findings elucidate the dynamics between Fe(III) incorporation in LDH and ferrihydrite precipitation, governed by pH-dependent solubility and charge-balance constraints.
研究领域:
无机化学
·
材料科学
·
环境地球化学
·
水泥化学
·
固体化学
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高影响因子
危险品化学品经营许可证（带存储）