SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Xiaoling Ma,Wenlong Wang,Chenggong Sun,Hui Li,Jing Sun,Xin Liu
In light of the promising merits of large surface area, uniform pore size, and tunable functional groups, metal-organic frameworks (MOFs) have great potential to be utilized for adsorbing volatile organic compounds (VOCs). In this study, three Fe-based MOFs, MIL-100(Fe), MIL-101(Fe), and MIL-53(Fe), were synthesized systematically and used to adsorb a typical VOC, toluene. Static adsorption, dynamic breakthrough curves , and adsorption kinetics were conducted to assess the adsorption performance. Additionally, the surface functional groups, pore structure, and morphology were systematically characterized by means of XRD , SEM, XPS, FTIR and N 2 adsorption-desorption analyses to reveal the cause of the difference in adsorption of these Fe-based MOFs. The results revealed that the maximum equilibrium adsorption capacity of 663 mg/g was achieved by MIL-100(Fe) with the highest specific surface area and pore volume. The dynamic adsorption of toluene on MIL-100(Fe) was in accordance with the pseudo-first order kinetic model and the Langmuir isothermal model. The formed π-π stacking interaction between organic ligands and the benzene ring in the MIL-100(Fe) cluster is the primary adsorption mechanism based on XPS analysis. Moreover, MIL-100(Fe) was easily regenerated via microwave irradiation with a negligible adsorption capacity decrease after three cycles. This work highlights the feasibility of hierarchical porous Fe-based MOFs as toluene adsorbents and promotes the application of MOFs in the field of pollution control .
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Mingxuan Fu,Guyang Ning,Jiaxian Liu,Qi Zhang,Yuena Sun,Xinyu Fan,Haiyang Wang,Haijun Lu,Yufan Zhang,Huan Wang
What is essential to solving energy scarcity problems is that develop the high activity, durable and non-noble metal-based dual-functional electrocatalysts for hydrogen evolution reactions (HER) and oxygen evolution reactions (OER). In this work, a series of core-shell structure M@Fe–Cu-GR nanocubes (NCs) are prepared. In the prepared process, the bimetallic FeCu prussian blue analogues (PBA) is used as precursor, transition metals ions Co 2+ and Ni 2+ are introduced into the FeCu-PBA using the exchange of potassium ions with other metal ions , and then the FeCu-PBA are successfully loaded on the graphene oxide (GO) employed the attraction of opposite charges between polydiallyldimethylammonium chloride (PDDA) and GO. Electrochemical tests show that the Tafel slope of Co–Ni@Fe–Cu–GR NCs for HER and OER are 60 and 82 mV dec −1 , respectively, and Co–Ni@Fe–Cu–GR NCs shows excellent performance in long-term stability test.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 5
·053505
·
IF 4.386
Yanfang Song,Jinxiong Wu,Jiliang Zheng,Yiwei Sun,Andrei Ivanets,Guangming Du,Xintai Su
The doping of multiple heteroatoms can improve the electrochemical properties of carbon substrates. However, in existing studies, carbon, iron and nitrogen sources are generally mixed directly and then pyrolyzed for secondary activation. This tends to form aggregates of metal particles or metal oxides and requires the consumption of large amounts of alkali and energy. Therefore, there is an urgent need to develop an environmentally friendly technology capable of uniformly doping iron and nitrogen into carbon materials. In this work, porous Fe–N–C composites were prepared at 600 °C using potassium humate (HA-K) obtained from cotton straw by low-temperature pyrolysis as the carbon source, and urea-iron complexes formed by the pre-coordination of urea and Fe as the iron and nitrogen sources. In the absence of secondary activation, the best sample Fe-NHPC-2 had a good mesoporous structure with high specific surface area (889. 01 m2 g−1). It had a high specific capacitance of 256.8 F g−1 at a current density of 0.5 A g−1. The capacitance retention was 92.6% after 10,000 cycles at a current density of 10 A g−1. In the symmetric supercapacitor application, the energy density reached 33.16 Wh kg−1 when the power density was 600.2 W kg−1.
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高影响因子
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART A-TOXIC/HAZARDOUS SUBSTANCES & ENVIRONMENTAL ENGINEERING
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2021
·
IF 2.269
Peng Zhou
A new material, polyacrylic acid-b-polyptyrene (PAA-b-PS) covered Ni/Fe nanoparticles (PAA-b-PS-nZVI-Ni), was developed and evaluated for the selective dechlorination of 1,1,1-trichloroethane (1,1,1-TCA) in the presence of potential interferents. The average size of the PAA-b-PS coated Fe/Ni bimetallic nanoparticles was approximately 50 nm, which resulted from agglomeration prevention by PAA-b-PS. The removal efficiency of 1,1,1-TCA by an optimal dose with a 1.0 g/L Fe/Ni (Ni/Fe = 2 wt%) and 0.5 g/L PAA-b-PS-coated concentration was higher (87.5%) than that of bare Fe/Ni (60%). The pseudo-first-order rate constant (Kobs) of 1,1,1-TCA removal by PAA-b-PS-nZVI-Ni was 0.0142 min−1 within 240 min. Comparatively, the Kobs values of 1,1,1-TCA removal by other materials (Fe, pure bimetallic Fe/Ni, PAA-b-PS-Fe) were only 0.003, 0.0052 and 0.0103 min−1, respectively. The 1,1,1-TCA removal efficacy by PAA-b-PS-nZVI-Ni showed no obvious gap regardless of pH or various common inorganic anions (NO3−, HCO3− and SO42−) at different concentrations. However, humic acid (HA) had great influence on the degradation of 1,1,1-TCA. In conclusion, PAA-b-PS-covered Ni/Fe nanoparticles with its selectivity high effectiveness could be used as one remedial agent for the degradation of 1,1,1-TCA in water.
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CATALYSIS TODAY
·
2020
·
IF 5.825
Rong Wang,Chizhong Wang,Sihan Yin,Yue Peng,Jianjun Chen,Yanxi Deng,Junhua Li
Nickel iron (oxy)hydroxide (NiFeO x H y ) is among the most active electrocatalysts for oxygen evolution reaction (OER) in the alkaline media. Development of new design strategy for NiFeO x H y electrode with respect to intrinsic activity and number of active species is highly attractive. Here we report a hierarchical fabrication for NiFeO x H y electrode towards efficient oxygen evolution. Three-dimensional mesoporous NiO was initially prepared and reduced to a polycrystalline Ni metal framework. Despite the poor OER activity for Ni-based catalyst, the incorporation of surface Fe species induced a notably high current density for the oxygen evolution. The results indicated that the Fe species, located at outer surface region, played a key role as the OER active sites. It is also found that the surface of metallic Ni was reconstructed to (oxy)hydroxide phase with ease compared to NiO. As a result, a heterostructure composed of an OER-active NiFe (oxy)hydroxide shell and an electron-conductive Ni core was formed. In this fabricated NiFeO x H y /Ni catalyst, the promoted intrinsic activity, number of active sites and charge-transfer ability all taken into account contribute to an efficient OER process.
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Journal of Energy Chemistry
·
2024
·
IF 14
Shiyu Li,Jin Yan,Meihuan Liu,Hui Su
The electrochemical conversion of nitrate, a widespread water pollutant, into valuable ammonia represents a green and decentralized approach to ammonia synthesis. However, the sluggish multielectron-proton coupling path and the low reactive species (nitrate and proton) concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction (NitRR). Herein, we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide (denoted as Fe-rGO), with a superior ammonia production rate of 47.815 mg h −1 mg −1 cat and a high Faraday efficiency (FE) of 96.51% at an applied potential of −0.5 V. It also delivers a robust stability with FE above 90% under a current density of 250 mA cm −2 for 50 h. In situ X-ray absorption spectroscopy reveals that the FeO x is dynamically translated to Fe 0 site concurrently with the enhancement of the NH 3 production rate, suggesting the Fe 0 site as hydrogenation active center. The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR, but also protects the iron species and ensures their stability during electrolysis. The Zn-NO 3 − battery demonstrates an impressive FE of 88.6%, highlighting its exceptional potential for practical applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Jiami Ma,Zhixin Hu,Weihong Guo,Cheng Ni,Pan Li,Bosheng Chen,Songhua Chen,Jinlong Wang,Yanbing Guo
Ground−level ozone (O 3 ) pollution poses a significant threat to both ecosystem sustainability and human health. The catalytic decomposition of O 3 presents as a promising technology to address the issues of O 3 pollution. This study undertook the synthesis of various functionalized metal−organic framework (MOF) catalysts ( i.e., X-MIL-53(Fe) (X = H, NH 2 , NO 3 )) to delve into the influence of ligand functional groups on skeletal structure and catalytic efficacy, particularly focusing on unraveling the mechanism of O 3 catalytic decomposition under humid conditions. NH 2 -MIL-53(Fe) catalyst achieved complete O 3 decomposition under ambient temperature and high humidity conditions (RH=75 %), exhibiting a reaction rates (mol·m −2 ·s −1 ) 129 and 10.5 times greater than that of MIL-53(Fe) and NO 2 -MIL-53(Fe). The NH 2 group promotes electron flow within the backbone towards the hydroxyl group (OH) linked to Fe atom. In humid O 3 , H 2 O molecules augment the interaction between O 3 and NH 2 -MIL-53(Fe), and OH is converted to·O 2 − after deprotonation, promoting O 3 decomposition. Additionally, leveraging three−dimensional (3D) printing technology, a monolithic catalyst for O 3 decomposition was prepared for application. This study not only advances understanding of the mechanisms underlying O 3 decomposition but also offers practical solutions for addressing O 3 pollution at humid conditions.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shengfeng Yang,Qingchao Xiao,Bin Li,Tao Zhou,Qihong Cen,Zewei Liu,Yue Zhou
Heavy metal contamination, particularly by lead and cadmium, poses a significant environmental challenge. Indiscriminate disposal of crop residues exacerbates environmental concerns. In this study, broad bean straw was utilized to produce biochar (BC), and further modifications were made using FeCl 3 -6 H 2 O and KMnO 4 to obtain Iron-Manganese Modified Biochar (FMBC) for remediating cadmium and lead-contaminated soil. Results show that both BC and FMBC increased soil pH, available phosphorus, and potassium compared to the control groups. Adding 5 % BC led to a notable reduction of 60.98 % in available cadmium and 51.63 % in available lead. Simultaneously, FMBC decreased active cadmium and lead by 57.51–73.73 % and 52.25–69.87 %, respectively. Furthermore, FMBC decreased the content of cadmium and lead in the unstable state while increasing content in the residual state, demonstrating its ability to reduce accumulation in plant tissues. FMBC adsorption mechanisms primarily involve surface complexation and co-precipitation, where oxygen-containing functional groups form stable complexes with free cadmium and lead ions. In conclusion, FMBC proved to be an effective, environmentally friendly soil remediation agent with strong adsorption capabilities and a prolonged shelf-life. This provides a promising solution to alleviate the pollution of heavy metals such as cadmium and lead in soil.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yuqi Li,Yue Zhang,Zhiyuan Wang,Chengxu Zhang,Fanming Meng,Jianqiang Zhao,Xinpei Li,Jue Hu
Metal-Organic Frameworks (MOFs) materials with unique properties have attracted much attention in various fields. However, the limited number of active sites and the time-consuming synthesis process hinder their widespread application. Herein, this work demonstrates the first preparation of highly efficient and stable MOF (Fe-MOF-U) catalysts with enhanced specific surface area , morphology and active sites, through ultrasonic-assisted solvothermal method for oxygen evolution reaction (OER) electrocatalysis . The results show that the crystal size of Fe-MOF-U decreases significantly, and the specific surface area and pore size increase. In addition, many oxygen vacancies are produced in the crystal, making the reaction intermediates easier to form and thus improving the catalyst's oxygen evolution performance. The overpotential of Fe-MOF-U catalyst at 10 mA cm −2 is 221 mV, which is lower than that of the conventional solvothermal synthesized Fe-MOF-S (237 mV). Furthermore, the turnover frequency of the Fe-MOF-U catalyst is 3.32 s −1 at the overpotential of 300 mV, which is 5 times higher than that of Fe-MOF-S (0.70 s −1 ). In situ Raman and methanol molecular probe tests indicate a weakened adsorption of *OH on the Fe-MOF-U surface. DFT calculations are consistent with the characterization results, both proving that the ultrasonic-assisted solvothermal method can generate specific oxygen vacancy (μ 3 -O defect) in Fe-MOF-U which improved OER performance. This study provides a new idea for the morphology controlling and defect introduction of MOF and a new approach for its application.
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高影响因子
Industrial Chemistry & Materials
·
2024
·
IF 0
Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu
Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 6
·2715-2723
·
IF 6.482
Xiaojing Feng,Zhongnan Guo,Xiaoxiao Yan,Jun Deng,Dan Wu,Zijing Zhang,Fan Sun,Wenxia Yuan
Metal phosphorus trichalcogenides (MPX3) are of great interest since these layered materials exhibit wide applications in optical, electrical and magnetic fields. An effective chemical intercalation route for MPX3 which could regulate their physical properties, however, is still lacking. In this work, we show that the liquid ammonia method is an efficient route to co-intercalate alkali metals and NH3 molecules into the gaps in FePS3. After intercalation, the interlayer distance is significantly enlarged by ∼3 Å while the monoclinic lattice (C2/m space group) is still maintained. The structure refinement and EDS measurement suggest that intercalation does not induce any Fe vacancy, thus leading to electron transfer from the alkali metal to [FePS3] layers. Interestingly, magnetic susceptibility shows that the intrinsic anti-ferromagnetic transition in the FePS3 matrix is completely suppressed by this intercalation, whereas a spin-glass state is observed in A(NH3)xFePS3 (A = Li, K) in the lower temperature range (<50 K). The intercalation described in this work is reversible: the alkali metal can be easily de-intercalated using a two-step route and the anti-ferromagnetism reappears accordingly. Meanwhile, the liquid ammonia method is also shown to be efficient at intercalating other MPS3 materials (M = Mn, Co, Ni). Our work not only enriches the intercalation chemistry in the MPX3 system but also provides an excellent route to regulate the magnetic properties of these layered materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Qiang Zhao,Dandan Li,Guofeng Gao,Wen Yuan,Genyan Hao,Jinping Li
We describe a novel nanostructured iron oxide catalyst film electrodeposited from iron(II) triflate under mild conditions (room temperature, atmospheric pressure, and near-neutral solution) that can catalyze water oxidation in potassium carbonate solution. The structure, morphology, composition, and catalytic activity of the catalyst were characterized by X-ray diffractometry, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical measurements. The results indicate that nanostructured iron oxide is an active electrocatalyst for water oxidation at higher catalytic current and low overpotential.
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高影响因子
危险品化学品经营许可证（带存储）