ACS Catalysis
·
2026
·Vol. 16
·期 20
·20616-20627
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IF 13.6
Yuan Jingkang,Zhao Chao,Jin Yu,Hou Qilin,Cui Zhi,Tan Daolin,Ou Honghui,Yan Xiaoqing,Yang Guidong
The electrocatalytic co-reduction of nitrate (NO 3 − ) and carbon dioxide (CO 2 ) into urea represents a potential avenue for achieving efficient urea production. However, this process involves intricate C–N coupling reactions and faces a severe kinetic mismatch between the reduction pathways. This disparity typically leads to a disproportionate coverage of key C- and N-containing intermediates on the catalyst surface, resulting in dominant competitive side reactions. Herein, we report the design of a heterogeneous FeNi@AC catalyst that integrates isolated Fe single atoms and Fe–Ni dual-atom sites at the atomic scale, enabling the efficient conversion of NO 3 − and CO 2 into urea. Combined experimental and theoretical investigations reveal that the isolated Fe single-atom sites retain high nitrate reduction capability. Crucially, the introduction of Ni induces an electronic reconfiguration of the Fe center, which significantly lowers the energy barrier for CO 2 activation (from 0.7 eV to 0.1 eV). This activation effectively bridges the kinetic gap between C- and N-species. Consequently, the FeNi@AC catalyst achieves a urea yield rate of 13.6 mmol g –1 h –1 and a Faradaic efficiency of 51.7% at –0.8 V (vs RHE). This work not only presents an active catalyst for urea synthesis but also provides a site-specific regulation strategy for designing multifunctional atomic-site catalysts tailored for complex tandem reactions.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Wenlong Zhang,Huanxin Li,Xiaohui Ning
The Fe/FeCl2-Graphite molten salt battery is a promising technology for large-scale energy storage, offering a long lifespan, a low operating temperature (<200 °C), and cost efficiency. However, its practical applications are hindered by the lack of a scalable preparation approach and insufficient redox stability in the Fe/FeCl2 electrode. Our study introduces an electrochemical anodic electrolysis (EAE) strategy, employing the anodic process (Fe → Fe2+) in an Al|AlCl3/NaCl/LiCl|Fe electrolysis system for the Fe/Fe2+ negative electrode in the Fe/FeCl2-Graphite battery. The EAE strategy forms an oxidized film, preventing incipient dissolution in the electrolyte and addressing redox stability issues with FeCl2 as the active substance. The Fe/Fe2+ negative electrode prepared by the EAE strategy exhibits a stabilized capacity of 0.72 mAh/cm2 after 7000 cycles at 5 mA/cm2, with a lower polarization level (∼29 mV) compared to FeCl2 as the active component. The flexibility of the EAE strategy is validated in both galvanostatic and potentiostatic processes, with a discharge capacity of 14 mAh after 1000 cycles, a capacity retention rate of 85%, and a Coulombic efficiency of 98% in the potentiostatic anodic electrolysis Fe/Fe2+ electrode. The scalability and reliability of the EAE strategy are further demonstrated in capacity-expanded Fe/FeCl2-Graphite batteries, reaching a discharge capacity of 155.1 mAh after 1000 cycles at 130 mA, with a capacity retention rate of 94%. For the first time, we showcased an EAE approach capable of producing Fe/Fe2+ electrodes at a rate of about 68.6 m2 per day. Additionally, we successfully assembled an Fe/FeCl2-Graphite battery at about a 0.42 ampere-hour level, paving the way for the scalable application of Fe/FeCl2-Graphite batteries.
研究领域:
能源材料
·
电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Peng Huang,Peng Zhang,Cuiping Wang,Jingchun Tang,Hongwen Sun
Persulfate-based (PS-based) advanced oxidation process is a promising technology for degradation of organic pollutants . PS activation needs efficient and economical catalysts and heterogeneous Fe-carbon composites are competitive. Herein, novel N-doped biochar-loaded nanoscale zero-valent iron (nZVI) composites (Fe@N-BC) were synthesized and evaluated for PS activation. Detailed characterization data indicated that graphitic and pyridine N structures were introduced by N-doping, which enhanced the anchoring, dispersion and loading of amorphous nZVI on biochar. Remarkably, the optimized Fe@N-BC material, Fe@N 2 -BC 900 , presented excellent catalytic performance for PS activation for lindane removal. The N-doped defects in biochar acted as reactive bridges and accelerated the electron transfer between nZVI and PS, showing strong synergistic effects toward nZVI. O 2 • − and 1 O 2 were the dominant active species in catalytic systems. Additionally, Fe@N 2 -BC 900 catalyst showed effectiveness over a wide pH range for lindane removal. This work provides a new approach to the rational design and application of Fe@N-BC for persulfate activation in pollution control, which is certified by deep exploration of reaction mechanism.
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ACS ES&T Water
·
2020
·
IF 0
Mingyue Zhao,Zhicheng Cui,Liang Fu,Fabrice Ndayisenga,Dandan Zhou
The slow reduction of Fe(III) to Fe(II) in electro-Fenton technology limits pollutant removal and causes Fe sludge production. This study hypothesizes that Shewanella, a dissimilatory iron-reducing bacteria, can accelerate the iron reduction of the Fenton reaction. A Shewanella biofilm coupled with Fe2O3 coated electrode (F/S) was used to drive the electro-Fenton reaction, and compared the results with the singlet Fe2O3 (F) anode and Shewanella biofilm anode (S). Meanwhile, dissolved oxygen (DO) is studied as an important influencing factor. The suitable DO was verified at ∼2 mg/L, phenol removal of F/S was 67% higher than that of the sum of three other singlet systems. The chemical oxygen demand (COD) removal was 72% and 50% higher than that of F and S, respectively. F/S corrosion current (Icorr) was 6.3 times higher than F, and induced hematite to transform into Fe2PO5 and FeOOH on the anode. Long-term operation showed that phenol was almost 100% removed for F/S; COD removal was generally 20% higher than F; thus, the toxicity of the effluent could be significantly decreased. The total Fe loss did not exceed 10% at the end of operation. This paper provides a feasibly novel method for electro-Fenton reaction, by employing Fe-reducing bacteria.
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Nano-Micro Letters
·
2020
·Vol. 12
·期 1
·1-16
·
IF 12.264
Deng Baiwen,Xiang Zhen,Xiong Juan,Liu Zhicheng,Yu Lunzhou,Lu Wei
Sandwich-like laminated Fe&TiO 2 @C nanocomposites were successfully prepared from the MXene–MOFs hybrids.
A broad effective bandwidth of 6.5 GHz at a thickness of only 1.6 mm was achieved.
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HYDROMETALLURGY
·
2020
·
IF 3.338
Xintao Yi,Guangsheng Huo,Wei Tang
The extraction of Fe(III), Ni(II) and Co(II) from a Ni(II)-Co(II) solution containing Fe(III) was analyzed in a chloride medium using a mixed extractant consisting of 50% ( v /v) tributyl phosphate (TBP), 20% (v/v) 2-octanol and 30% (v/v) kerosene. The extraction of 0.5 mol/L Fe(III) in 4 mol/L hydrochloric acid reached 97%, and the consumption of chloride ions was investigated. Nickel(II) ions were not detectably extracted by TBP, with an inclusion of <1.1%. Compared with Fe(III), TBP extracted only a small amount of Co(II). The iron complexes formed by TBP and 2-octanol were [H 2 FeCl 4 · 2TBP] and [H 2 FeCl 4 · 5(2-octanol)], and the possible compositions of Co-containing extracts were [H 2 CoCl 4 · 2TBP] and [H 2 CoCl 4 ] · n[2-octanol]. An industrial process consisting of two-step extraction was designed to achieve the separation of Co(II) and Fe(III), resulting in a decrease in the Fe/Co mass ratio from 0.46 to <3.5 × 10 −4 in the raffinate.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Zhuoqian Li,Kai Li,Shuanglong Ma,Bingjun Dang,Yi Li,Haichao Fu,Jinge Du,Qingxiang Meng
A convenient and efficient method to fabricate isolated Fe single-atom catalysts deposited on Myriophyllum aquaticum -based biochar (ISA-Fe/MC) is reported for peroxymonosulfate-based organics degradation. Firstly, the Fe nanoparticles anchored on the hierarchical porous biochar (nano-Fe/MC) can be obtained by utilizing K 2 FeO 4 as a synchronous activation and graphitization agent. Subsequently, ISA-Fe/MC was achieved by HCl etching of nano-Fe/MC to remove the excess Fe nanoparticles. Compared with nano-Fe/MC, ISA-Fe/MC demonstrated outperformed catalytic capacity towards PMS activation for phenol degradation. The combination of super high surface area, hierarchical porous structure, graphitization structure and atomically dispersed Fe species should be responsible for prominent catalytic oxidation ability and outstanding resistance to common anions and humic acid. Based on the chemical scavengers, EPR experiments and electrochemistry tests, the SO 4 •– dominated radical degradation pathway for nano-Fe/MC and electron transfer reigned non-radical degradation pathway for ISA-Fe/MC was revealed. In contrast to nano-Fe/MC, density functional theory calculations demonstrated the enhanced density of states around Fermi level in ISA-Fe/MC meaning the increased catalytic performance and more electron transfer between single-atom Fe to adjacent graphitic C and N which could serve as electron transfer channel for PMS activation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Peng Zhou,Jing Zhang,Zhaokun Xiong,Yang Liu,Xiaowei Huo,Xin Cheng,Wenshu Li,Feng Cheng,Yongli Zhang
Hydroxylated C 60 Fullerene (Fullerol) induced photochemical production of reactive oxygen species (ROS, e.g. singlet oxygen ( 1 O 2 ) and hydroxyl radical ( OH)) is a slow process, and the role of its surface groups other than high water-solubility is still lack of investigation. In this study, we demonstrate Fullerol can promote Fe(III)/Fe(II) cycles to degrade dimethyl phthalate (DMP) in Fe(III)/H 2 O 2 Fenton system as both an electron donor and an electron-transfer mediator. At acidic condition, the formation of carbonyl and carboxyl via pinacol rearrangement and subsequent keto-enol isomerization can produce cage-opened structure of Fullerol, resulting in the pH-dependent formation of Fe(III)-Fullerol complex. Two pathways of Fe(II) recovery via intramolecular electron transfer of Fe(III)-Fullerol complex to enhance Fe(III)/H 2 O 2 Fenton oxidation were proposed: 1) Fullerol direct reduces Fe(III) into Fe(II) as an electron donor in dark, and it was strongly enhanced under visible light irradiation; 2) Fullerol mediates electron transfer from electron donor (e.g. hydrogen peroxide and organics) to Fe(III) in visible light condition. Furthermore, DMP degradation pathway was proposed based on variation of main intermediates.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Jinzhao Wang,Di Huang,Fengxia Chen,Jianhua Chen,Hongyu Jiang,Yifan Zhu,Chuncheng Chen,Jincai Zhao
Fe(III) and carboxylic acids are common compositions in atmospheric microdroplet systems like clouds, fogs, and aerosols. Although photochemical processes of Fe(III)–carboxylate complexes have been extensively studied in bulk aqueous solution, relevant information on the dynamic microdroplet system, which may be largely different from the bulk phase, is rare. With the help of the custom-made ultrasonic-based dynamic microdroplet photochemical system, this study examines the photochemical process of Fe(III)–citric acid complexes in microdroplets for the first time. We find that when the degradation extent of citric acid is similar between the microdroplet system and the bulk solution, the significantly lower Fe(II) ratio is present in microdroplet samples due to the rapider reoxidation of photogenerated Fe(II). However, by replacing citric acid with benzoic acid, no much difference in the Fe(II) ratio between microdroplets and bulk solution is observed, which indicates distinct reoxidation pathways of Fe(II). Moreover, the presence of •OH scavenger, namely, methanol, greatly accelerates the reoxidation of photogenerated Fe(II) in both citric acid and benzoic acid situations. Further experiments reveal that the high availability of O2 and the citric acid- or methanol-derived carbon-centered radicals are responsible for the rapider reoxidation of Fe(II) in iron–citric acid microdroplets by prolonging the length of HO2•- and H2O2-involved radical reaction chains. The results in this study may provide a new understanding about iron–citric acid photochemistry in atmospheric liquid particles, which can further influence the photoactivity of particles and the formation of secondary organic aerosols.
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ACS Nano
·
2019
·
IF 13.903
Xiang Ao,Wei Zhang,Zhishan Li,Jian-Gang Li,Luke Soule,Xing Huang,Wei-Hung Chiang,Hao Ming Chen,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
Single-atom catalysts (SACs) have emerged as one of the most promising alternatives to noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). While SACs can offer notable benefits in terms of lowering overall catalyst cost, there is still room for improvement regarding catalyst activity. To this end, we designed and successfully fabricated an ORR electrocatalyst in which atomic clusters are embedded in an atomically dispersed Fe–N–C matrix (FeAC@FeSA–N–C), as shown by comprehensive measurements using aberration-corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential of FeAC@FeSA–N–C is 0.912 V (versus reversible hydrogen electrode (RHE)), exceeding that of commercial Pt/C (0.897 V), FeSA–N–C (0.844 V), as well as the half-wave potentials of most reported non-platinum-group metal catalysts. The ORR activity of the designed catalyst stems from single-atom active centers but is markedly enhanced by the presence of Fe nanoclusters, as confirmed by both experimental measurements and theoretical calculations.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Haoran Dong,Yujun Cheng,Yue Lu,Kunjie Hou,Lihua Zhang,Long Li,Bin Wang,Yaoyao Wang,Qin Ning,Guangming Zeng
This study examined the toxicities of Fe/Ni and starch-stabilized Fe/Ni (S-Fe/Ni) nanoparticles (NPs) toward Escherichia coli . The inactivation of E. coli by Fe/Ni NPs was concentration- and time-dependent. Fe/Ni NPs exhibited a stronger toxicity than the bare Fe 0 NPs (i.e., Ni = 0 wt%), revealing that the loading of Ni increased the toxicity of Fe 0 NPs. However, there was no positive correlation between Ni content and the toxicity of Fe/Ni NPs when Ni content increased from 1 wt% to 5 wt%. The starch coating could alleviate the toxicity of Fe/Ni NPs, depending on starch concentration. Transmission Electron Microscopy analysis demonstrates that membrane disruption and cellular internalization of NPs occurred for E. coli after exposure to the Fe/Ni NPs. The NPs might have reacted with the carboxyl, ester and amine groups on the cell surface, as indicated by the Fourier Transform Infrared Spectroscopy analysis. However, the S-Fe/Ni NPs did not cause obvious membrane disruption of the cells due to the effect of starch coating, which inhibited the close contact of NPs with cells by providing electrostatic repulsion and steric hindrance. Besides, the addition of N-Acetyl-L-cysteine, as a potent scavenger for reactive oxygen species (ROS), remarkably reduced the toxicities of both Fe/Ni and S-Fe/Ni NPs, which indicated that the ROS-induced oxidative stress should be the primary mechanism for the inactivation of E. coli . The aging experiments evidenced that both Fe/Ni and S-Fe/Ni NPs would lose their toxic potential over time, posing less threat to the environment in the long term.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
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