APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Shuhao Li,Feng Wang,Derrick Ng,Simon James,Zongli Xie,Boxiong Shen
Supported catalysts have been extensively investigated and implemented in the industry due to their cost-effectiveness and promising catalytic performance. However, due to the general inert nature of the support itself, its role in the catalyst performance is often neglected and therefore not well understood despite the consideration of the physical properties of the support. This study applies the concept of electronic metal-support interaction (EMSI) to explore the impact of various supports on the active metals in Fe-Ni-based catalysts for the CO-selective catalytic reduction reaction. Through density functional theory calculations and several advanced characterizations, it can be confirmed that the EMSI effect can modify the valence states of active metals and foster interaction between different active metals, thereby influencing the reactant adsorption and catalyst performance greatly. These findings highlight the significant impact of the support on the chemical states of active metals, having far-reaching implications for designing and optimizing the supported industrial catalysts.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jianyue Yan,Peng Liu,Jiawen Li,Hao Huang,Shengfu Tong,Wenbo Song
The electrocatalytic nitrate reduction reaction to ammonia (NRA) offers a promising alternative to traditional ammonia synthesis methods. In nature, enzymes containing molybdenum and iron sites catalyze the reduction of nitrate and nitrite ions. Drawing inspiration from these enzymes, we synthesized a carbon-coated nano-octahedra of FeMo-based nitride (FeMoN@C NO) by pyrolyzing phosphomolybdic acid hydrate (POM) doped Fe-NH 2 -MIL-101 to catalyze NRA. Experimental results demonstrate that in an alkaline environment, FeMoN@C NO exhibits a suitable hydrogen evolution reaction (HER) capacity, and the protons or hydroxyls produced effectively facilitate the hydrogenation reaction in the ammonia synthesis process. Additionally, the introduction of Mo increases the number of active sites and effectively reduces the thermodynamic barrier in NRA, thereby enhancing the rate of ammonia synthesis. As a result, FeMoN@C NO displays outstanding NH 3 Faradaic efficiency (FE) of 98.2 % and an NH 3 yield of 434.16 µmol/h cm −2 . Building upon the excellent electrocatalytic properties of FeMoN@C NO, a new Zn-nitrate battery system is assembled in this work, which exhibits an outstanding peak power density of 3.23 mW cm −2 and an FE of 91.58 % for NH 3 production. This work provides a new perspective for designing enzyme-mimicking nitrate reduction catalysts and broadens the application of Zn-based batteries.
研究领域:
电化学
·
材料科学
·
催化
·
能量存储
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenxuan Zhou,Xiaoyong Mo,Cham Wah Cheung,Edmund C.M. Tse
At present, over 95 % of H 2 O 2 is produced via the anthraquinone process that requires large infrastructure, generates organic pollution, and poses safety issues. Electrochemical H 2 O 2 generation through oxygen reduction can serve as an alternative, reliable, and decentralized production method if affordable and high-performance electrocatalysts can be developed. Herein, a two-step process is used to prepare an Fe-based complex as a non-precious metal electrocatalyst to facilitate oxygen reduction reaction (ORR) and produce an alkaline H 2 O 2 solution. The Fe complex of benzene-1,3,5-tricarboxylate (FeBTC) is first synthesized using a hydrothermal method and then activated via a pulsed laser treatment process that is optimized via the Taguchi method. The pulse-laser-treated FeBTC (PL-FeBTC) lowers the H 2 O 2 electrosynthesis overpotential by 50 mV at −0.1 mA/cm 2 and exhibits a 25 % increase in H 2 O 2 product selectivity at 0.4 V vs. RHE. The experimental results indicate that the O 2 -to-H 2 O 2 turnover frequency and electrocatalytic yield of the Fe-based metal–organic framework are enhanced simultaneously through solid-to-solid pulsed laser conversion. Through a series of X-ray photoelectron spectroscopy, elemental analysis, Raman spectroscopy, X-ray absorption spectroscopy, and control atmospheric experiments, the origin of the improvement in catalytic performance is rationalized through the formation of an oxo-bridge across the di–Fe active site via an oxygen-doping mechanism, thus providing a systematic laser methodology for precise structure-performance tuning. Beyond H 2 O 2 generation, this study further lays the foundation for the development of cost-effective and scalable electrocatalysts that are central to other commodity manufacturing and sustainable resourcification processes.
研究领域:
材料科学
·
电化学
·
催化
·
可持续化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Limeng Yang,Wendou Chen,Cuihong Sheng,Hailiang Wu,Ningtao Mao,Hui Zhang
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are encouraging methods for wastewater treatments, but the recycling of used PMS activators in powder form from the wastewater treatment system is still problematic. In this paper, we designed a novel and highly effective carbocatalyst for PMS activation, which was achieved by pyrolyzing the hybrids of metal–organic framework MIL-101(Fe) and dicyandiamide immobilized on the surface of carbon cloth (CC), and a facile route for the preparation of fibrous catalysts was developed. The resultant CC loaded with Fe/N-codoped carbocatalyst exhibited desirable reusability and good stability for the degradation of organic dyes. The mechanism of the novel Fe/N-codoped carbocatalyst for PMS activation including the specific roles of N species and Fe-N binding was investigated. It was demonstrated in electrochemical impedance spectroscopy (EIS) results that the CC facilitated the electron transport of the carbocatalyst in AOPs. It was shown in the radical quenching and electron paramagnetic resonance (EPR) experiments that both the radical and non-radical pathways were accountable for the degradation of contaminants, and the non-radical path was principal. It was also evident in the X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results that pyridinic N and graphitic N were the main active species for PMS activation.
研究领域:
环境科学
·
催化
·
水处理
·
材料科学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Wei-Chang Chen,Xiao-Shuang Guo,Ze-Yu Liu,Chuan-Qing Huang,Jian-Shan Ye,Hai-Yang Liu,Xin-Yan Xiao
Fe-based nanoparticles encapsulated in carbon can effectively promote the ORR activity of the neighboring Fe–N x and prevent the dissolution of metal nanoparticles to ensure the long-term durability of catalysts. Herein, we employed a facile two step pyrolysis strategy to construct “plane-active sites” structure, namely FeO y nanoparticles embedded in carbon were loaded on two dimensional (2D) porous carbon with exposed abundant Fe–N x active sites (FeOy@C/Fe-N x /C). The optimized FeO y @C/Fe-N x /C catalyst with low Tafel slope (48 mV dec −1 ) and nearly-four-electron selectivity (3.91–3.97) showed excellent performance towards ORR with a more positive shift of 15 mV of half-wave potential (E 1/2 = 0.856 V) than that of commercial Pt/C (E 1/2 = 0.841 V) in alkaline solution, and also had a superior long-term stability and methanol resistance as compared with commercial Pt/C. The excellent electrochemical performance of FeO y @C/Fe-N x /C can be attributed to FeO y @C structure, exposed abundant Fe–N x active sites and two dimensional porous carbon with a large specific surface area.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yu-qiong Gao,Yan-yan Rao,Han Ning,Ju-xiang Chen,Qian Zeng,Fu-xiang Tian,Nai-yun Gao
The degradation of diclofenac (DCF), a commonly used nonsteroidal anti-inflammatory drug, by Fe 2+ /chlorine and Fe 2+ /PMS processes was comparatively investigated. The influencing factors of pH, Fe 2+ and oxidant dosage on DCF degradation efficiency were evaluated and optimized. Typically, with an initial solution pH of 5, an Fe 2+ dosage of 70 μM, and a chlorine or PMS dosage of 70 μM, the degradation efficiency of DCF using the Fe 2+ /chlorine and Fe 2+ /PMS processes reached 94.2% and 79.7%, respectively, within 10 min. Quenching tests indicated the coexistence of •OH and RCS in the Fe 2+ /chlorine system, and both SO 4 ●– and •OH were identified in the Fe 2+ /PMS system. In addition, Fe(IV) was also identified to participate in DCF degradation in two systems based on the oxidation of PMSO to PMSO 2 . The degradation products and pathways of DCF were elucidated by LC/TOF/MS analysis and DFT calculations. It was assumed that the degradation pathway of DCF involves hydroxylation, dechlorination, decarboxylation, cleavage of the C-N bond, and chlorine substitution. In addition, trichloromethane (TCM), dichloroacetaldehyde (DCAL), dichloroacetonitrile (DCAN) and trichloronitromethane (TCNM) were also detected in the Fe 2+ /chlorine process, and these chlorinated DBPs initially increased and then decreased with prolonged reaction time, indicating that Fe 2+ /chlorine is capable of controlling DBPs formation. Finally, the acute and chronic toxicity of DCF and its degradation products were evaluated by the ECOSAR program.
研究领域:
环境科学
·
化学工程
·
毒理学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Siqi Liu,Andrey M. Kuznetsov,Weiqing Han,Alexei N. Masliy,Gregory V. Korshin
Methylated arsenic species are ubiquitous in the environment and resistant to removal by conventional treatment technologies. This study addressed this challenge based on the examination of the removal of dimethylarsinic acid (DMA) in a system that combines zerovalent iron (ZVI) and powdered activated carbon (PAC). The removal of DMA in the ZVI/PAC system was compared to that by coagulation, adsorption, electrochemical and Fenton oxidations, and other conventional methods. While only the electrochemical oxidation using a PbO 2 /Sb-SnO 2 /Ti anode allowed removing up to 60% DMA at several hours-long treatment times, the removal of DMA in the ZVI/PAC system containing 10 g/L ZVI and 2.5 g/L PAC with an initial pH of 2.0 was 95% for a 30 min reaction time. Specific roles of PAC, ZVI and its oxidation products in DMA removal were examined based on the spectroscopic data and quantum chemical modeling for the DMA/Fe(II) and DMA/Fe(III) systems. These methods demonstrated the formation of moderately strong DMA/Fe(II) and DMA/Fe(III) complexation. These results and relevant kinetic data were interpreted to indicate that the removal of DMA is governed by the rapid generation of Fe 2+ ions released as a result of accelerated ZVI corrosion in the galvanic ZVI/PAC microcells and ensuing formation of DMA/ Fe 2+ complexes that are readily adsorbed by PAC.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yuxiang Mao,Jun Cheng,Hao Guo,Lei Qian,Jiacan Tu,Weijuan Yang
To enhance catalytic acid-base sites in ZIFs and efficiently promote conversion of microalgal lipids, a bifunctional catalyst with single-atom Fe-N 4 sites and Fe nanoparticles (NPs) was synthesized by pyrolyzing Fe-doped ZIF-8. Compared with ZIF precursors, Fe nanoparticles and coordinated Fe ions in Fe-N 4 sites enhanced Lewis acidity, while increased uncoordinated N atoms enhanced Lewis basicity. Therefore, the acidity of Fe-NC increased from 0.473 to 1.845 mmol/g, while basicity increased from 0.172 to 0.439 mmol/g. DFT calculations showed that the adsorption energies of acetic acid on the Fe–N 4 and Fe NP were −0.536 eV and −0.397 eV, respectively, exceeding that (-0.190 eV) on the Zn–N 4 site. The energy barriers for rate-determining steps over the Fe-N 4 and Fe NP were + 0.32 eV and + 0.21 eV, respectively, which were lower than that (+1.01 eV) over the Zn-N 4 site. The maximum biodiesel yield reached 98.3% over Fe-NC catalyst, higher than that (84.5%) over ZIF-8 catalyst.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 12
·5223-5231
·
IF 2.7
Tingli Ren,Yuanfeng Liu,Xiaoqiu Lin,Congju Li
The fairly low power density, mainly resulting from poor electroactive bacterial (EAB) adhesion and the sluggish extracellular electron transfer (EET) at the anode interface, constrains the practical implementation of microbial fuel cells (MFCs). Therefore, the properties of the anode material are considered to be a crucial factor for the long-term operational performance of MFCs. In order to enhance the power production performance of MFCs, an aerogel composed of Fe, N, and S co-doped carbon nanofibers (CNFs) and reduced graphene oxide (rGO) was employed as a high-performance anode material by electrospinning, high-temperature pyrolysis and freeze-drying. The doping of Fe, N and S elements induced the formation of abundant reactive sites on the CNFs, which enhanced the electrochemical performance of the anode and the EET process. The huge electroactive area of the samples facilitated the formation of dense biofilms. Therefore, an MFC with the FeS/Fe3C@NCNFs/rGO-modified anode achieved a maximum power density of 2792.56 mW m−2 and the highest output voltage of 0.658 V, both of which were significantly higher than those of the carbon cloth anode (773.97 mW m−2 and 0.443 V). Considering the great improvement in power production, it has considerable potential as a low-cost but high-performance anode material for MFCs.
研究领域:
材料科学
·
环境工程
·
电化学
·
生物技术
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 115
·94694-94701
·
IF 3.84
Xue-ming Lin,Yong-wen Ma,Yan Wang,Jin-quan Wan,Ze-yu Guan
Lithium iron phosphate (LiFePO4) was prepared and applied in the heterogeneous activation of persulfate (PS) for Orange G (OG) degradation in water. Scanning electron microscopy, X-ray diffraction, Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) were used to characterize the properties of the material before and after activation. The effects of several parameters on its catalytic activity were also investigated. It was found that the catalyst presented ultrafast activity for OG and other organic dye degradations. The results from XPS further suggested that the highly catalytic efficiency possibly involved the activation of PS to sulfate radicals as main radical meditated by the redox pair of Fe(II)/Fe(III) of LiFePO4/FePO4.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zheng Wang,Keizo Nakagawa,Kecheng Guan,Aiwen Zhang,Yasunao Okamoto,Atsushi Matsuoka,Eiji Kamio,Tomohisa Yoshioka,Hideto Matsuyama
s The stability of solvent-resistant nanofiltration (SRNF) membranes, such as integrally skinned asymmetric (ISA) and thin-film composite (TFC) membranes, in polar aprotic solvents must be improved if they are to meet increasingly complex industrial demands. The stability of the former membranes can be improved by forming crosslinked rigid chains, such as polybenzimidazoles and polyimides, but this requires time-consuming treatment processes. Conversely, the latter membranes are easy to fabricate but lack efficient active sites for crosslinking and structural rigidity. Herein, we present a fabrication strategy combining the characteristics of both types of membranes. We first utilize amino-functional porphyrins as polyaromatic units to form rigid polyamide networks by vacuum-assisted interfacial polymerization, simultaneously providing active sites for further crosslinking, which is accomplished by immersion in FeCl 2 /dimethyl sulfoxide (DMSO) solution to directly establish Fe-O-Fe bridges between porphyrin centers to form a stable network. The Fe-O-Fe-bridged porphyrin networks are solvent-stable in DMSO. Furthermore, they achieve outstanding molecular separation (96.2% rejection of methyl orange, 327 Da) and limited molecular-weight-cutoff change (from 360 to 420 Da) during alternating MeOH and DMSO filtration, along with long-term recovery efficiency (> 96.7% over seven days). Thus, our study provides a promising strategy for the facile development and fabrication of efficient, robust SRNF membranes.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2024
·Vol. 150
·期 6
·04024020
·
IF 1.6
Dawei Wang,Tingyue Chen,Yilan Jiang,Xinyang Cai,Yingying Li,Yuanyuan Chen,Guang Yang,Feng Pan
Promoting the Fe(II)/Fe(III) cycle efficiency is of wide interest for the broader applications of the Fenton process in water treatment sector. In this study, the alternating magnetic field (AMF) was employed to accelerate the reduction from Fe(III) to Fe(II). To achieve this purpose, a composite of nano-zero valence iron and NiFe2O4 was fabricated (denoted as Fe@NiFe2O4). Under the optimal reaction conditions, bisphenol A (BPA) was removed completely within 15 min by the Fe@NiFe2O4/H2O2 system in the presence of AMF, while only ∼60% was removed in the absence of AMF. The faster removal rate in the presence of AMF was ascribed to the elevated temperature caused by the inductive heating of Fe@NiFe2O4 (∼41°C according to the simulation). The simulator of the Fenton process was considered to be the leaked Fe(II) from the Fe part of the composite, as an equal concentration of Fe(II) (∼5.7 mg/L) resulted into a similar removal kinetic. However, the system with Fe@NiFe2O4 as the catalyst consumed less H2O2 in this process, indicating its different activation pathway from the conventional Fenton process. Electrochemical analysis confirmed that the AMF can generate the internal electric field within the composite particle. This field may facilitate the reduction from Fe(III) to Fe(II), which further benefitted the Fenton reactions.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）