Small
·
2018
·Vol. 14
·期 8
·1702827
·
IF 9.598
Erling Li,Fa Yang,Zhemin Wu,Yong Wang,Mingbo Ruan,Ping Song,Wei Xing,Weilin Xu
Herein, a type of Fe, N-codoped carbon electrocatalyst (FeN x /C, Fe-N-BCNT#BP) containing bamboo carbon nanotubes and displaying bifunctional high catalytic efficiency for both oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CO2RR) is reported. It shows high electrocatalytic activity and stability for both the ORR process with onset potential of 1.03 V RHE in alkaline and the CO2RR to CO with high faradic efficiency up to 90% and selectivity of about 100% at low overpotential of 0.49 V. For CO2RR to CO, it is revealed that Fe 3 C is active but the activity of FeN x centers is lower than that of C–N-based centers, contrary with that observed for ORR. Due to its low cost and high electrocatalytic performance for these two reduction reactions, the obtained catalyst is very promising for extensive application in future. The revealed huge activity difference of the same types of active sites for different reactions can efficiently guide the synthesis of advanced materials with multifunction.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 12
·1-10
·
IF 2.4
Wang Zhenzhen,He Shaofeng,Ji Xing,Fang Zefeng,Wang Jing
Transition metal nitrides (TMNs) have emerged as promising alternatives to commercial Pt/C in hydrogen evolution reaction (HER) owing to high conductivity and electronic structure similar to that of Pt. Nevertheless, the applications of TMNs-based catalysts are limited by the complex preparation processes. Developing highly efficient TMNs-based catalysts via simple and eco-friendly synthesis strategies still poses a substantial challenge. In the research, Ru/FeN x /C catalysts are in-situ synthesized through combining ion-exchange and confined pyrolysis strategies by leveraging the intrinsic Fe-N coordination structure of Prussian Blue. The Ru components are preferentially anchored adjacent to FeN x , forming abundant synergistic active centers. The contents of Ru and Fe in Ru/FeN x /C-900 are as low as 0.31 wt% and 0.05 wt%, respectively. The Ru/FeN x /C-900 attains a current density of 10 mA cm −2 at an overpotential of merely 15 mV in a 1.0 M KOH solution, exhibiting superior performance to the commercial Pt/C. The systematic experimental results unveil that the electron transfer between Ru and FeN x optimizes the distribution of active Ru and Fe-N x species, thereby accelerating the reaction kinetics and improving the catalytic activity. Graphical
研究领域:
材料科学
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电催化
·
能量转换
·
纳米材料
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106507
·
IF 4.386
Mengxue Huang,Ruimin Ding,Jie Yang,Wenwen Shi,Shufang Shi,Lifang Chen,Shanshan Liu,Xi Yin
Platinum group metal-free catalysts based on transition metal and nitrogen co-doped carbon materials are gaining attention for their applications in electrocatalysis. Nitrogen-coordinated metal sites (MNx) have been identified as the main active sites in PGM-free catalysts. Current synthetic approaches rely on the high-temperature treatment to introduce targeted electroactive MNx sites into the carbon matrix. In this study, we demonstrated the formation of MNx sites on Ni- and N-co-doped carbon templates via the solution-phase coordination with target metal ions, including Fe2+, Fe3+, and/ Co2+. The formation of MNx sites was confirmed via a combined approach of various physical characterization techniques, elemental analysis, and electrochemical analysis. The results indicate that the metal-vacancy-Nx sites in the template can coordinate with target ions to form electrochemically active MNx sites. By varying heat-treatment temperature, the amount of FeNx sites formed via coordination with Fe2+ ion can be tuned and correlated with the change of activity toward oxygen reduction reaction. The amount of MNx sites formed via solution-phase coordination with various ions followed the sequence of Co2+ > Fe2+ > Fe3+. These findings may further guide the future development of MNx-C electrocatalysts through this solution-phase coordination approach.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Green Energy & Environment
·
2021
·
IF 8.207
Siyuan Sun,Weijie Bao,Fan Yang,Xingru Yan,Yang Sun,Ge Zhang,Wang Yang,Yongfeng Li
A novel strategy was developed to fabricate FeN x -doped carbon quantum dots (Fe-N-CQDs) to detect Cu 2+ ions selectively as a fluorescence probe. The Fe-N-CQDs were synthesized by an efficient electrolysis of a carbon cloth electrode, which was coated with monoatomic iron-anchored nitrogen-doped carbon (Fe-N-C). The obtained Fe-N-CQDs emitted blue fluorescence and possessed a quantum yield (QY) of 7.5%. An extremely wide linear relationship between the Cu 2+ concentration and the fluorescence intensity was obtained in the range from 100 nmol L −1 to 1000 nmol L −1 (R 2 = 0.997), and the detection limit was calculated as 59 nmol L −1 . Moreover, the Fe-N-CQDs demonstrated wide range pH compatibility between 2 and 13 due to the coordination between pyridine nitrogen and Fe 3+ , which dramatically reduced the affection of the protonation and deprotonation process between H + and Fe-N-CQDs. It is notable that the Fe-N-CQDs exhibited a rapid response in Cu 2+ detection, where stable quenching can be completed in 7 s. The mechanism of excellent selective detection of Cu 2+ was revealed by energy level simulation that the LUMO level of Fe-N-CQDs (−4.37 eV) was close to the redox potential of Cu 2+ , thus facilitating the electron transport from Fe-N-CQDs to Cu 2+ .
研究领域:
分析化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Juejin Teng,Min Wang,Wenwen Zhou,Lina Geng,Yilin Wang,Mingbo Wu,Zhongtao Li
Atomic phosphorus doping creates Lewis-base “proton pump” sites that coordinate interfacial water, dramatically lower the water dissociation barrier (0.87 → 0.05 eV). • This targeted acceleration of the rate-determining step boosts the peak power density of Zn–air batteries to 183 mW·cm -2 . • Increases the open-circuit voltage and broadens the operational voltage window. Development of Fe-NC catalysts is fundamentally challenged by their performance decay in acidic media, originating from insufficient proton-coupled electron transfer kinetics and irreversible iron leaching. Herein, we transcend conventional electronic structure modulation by introducing a local interfacial pH tailoring strategy via atomic phosphorus doping. The incorporated P species, serving as Lewis-base sites, function as efficient “proton pumps”. They actively coordinate with interfacial water molecules via lone-pair electrons, which not only enhances H 2 O adsorption but also significantly weakens the O H bond, drastically reducing the water dissociation energy from 0.87 to 0.05 eV. This triggered water activation creates a unique proton-enriched interfacial microenvironment at the catalyst interface while maintaining an alkaline bulk electrolyte, a phenomenon directly visualized by in-situ Raman spectroscopy. The accelerated local proton supply promotes the rate-determining *OOH formation step, while the modulated electronic structure concurrently stabilizes the Fe-Nₓ centers, suppressing Fe dissolution to a remarkably low level. When deployed in a Zn-air battery, this synergistic mechanism enables the Fe-P-NC cathode to achieve a record-high power density of 183 mW·cm −2 . This work underscores the profound potential of active interfacial microenvironment engineering in breaking the activity–stability trade-off for advanced electrocatalysis.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shizong Wang,Jianlong Wang
In this study, the bimetallic and nitrogen co-doped biochar was prepared for peroxymonosulfate (PMS) activation to degrade emerging contaminants. Compared to single metal-doped biochar, bimetallic-doped biochar showed much higher catalytic activity. Iron and cobalt co-doped biochar (FeCo-BC) exhibited higher catalytic activity than iron and copper co-doped biochar (FeCu-BC). When FeCo-BC was used for PMS activation, sulfamethoxazole (SMX) could be completely removed within 10 min, with the degradation rate of 0.749 min −1 , which was 2.3 and 69.4 times higher than that of Fe-BC (0.333 min −1 ) and Co-BC (0.0108 min −1 ), respectively, demonstraing the synergistic effect of bimetallic co-doping. Meanwhile, the SMX mineralization efficiency reached 57.1 %. In the system of FeCo-BC/PMS, multi reactive species produced, in which hydroxyl radicals, sulfate radicals and high-valent metal-oxo mainly contributed to SMX degradation. The superior catalytic activity of FeCo-BC was attributed to the configuration of FeNx-CoNx. In five consecutive experiments, FeCo-BC showed good catalytic activity and stability. This study provides a way to the rational design of high efficient and stable PMS catalyst, which could be used in Fenton-like reaction to remove the emerging organic contaminants.
研究领域:
环境科学
·
催化材料
·
污染治理
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Hongmin Sun,Zhiyuan Ge,Yingru Wang,Donglai Li,Ruolin Peng,Ziliang Deng,Renjie Chang,Wenbo Dong,Chen Wen,Jingbo Li,Yeliang Wang,Shuailong Zhang,Juncai Dong,Yao Yang,Haibo Jin,Liang Cao,Zipeng Zhao
Breaking the known activity–stability trade-off is essential for the broad implementation of Fe–N–C catalysts in fuel cells. Here, we report the development of an atomically dispersed Fe–N–C catalyst with highly active FeNx sites on carbon support with dispersed graphitic microdomains (FeNx-Gmd), which were generated during the Fe3C-catalyzed graphitization. The introduction of graphitic microdomain makes the FeNx-Gmd exhibit outstanding oxygen reduction reaction activity when used as a cathode catalyst in practical fuel cells, with impressive peak power densities of 1.06 and 0.55 W cm–2 under 150 kPaabs H2/O2 and H2/air, respectively. Both power densities proved that the FeNx-Gmd were among the top five best-reported non-PGM-based catalysts. Theoretical calculations suggested the FeNx sites supported on carbon structure with fewer defects, corresponding to a higher graphitic degree, showing higher activity compared to the one with more defects. Moreover, the improvement in catalyst activity does not compromise stability since graphitic microdomains enhanced the corrosion resistance of the carbon support. As a result, after 10000 cycles of accelerated stability test, the FeNx-Gmd can still deliver a peak power density of 0.79 W cm–2 in the H2/O2 test, which was even higher than many catalysts at the initial stage. Unlike the reported strategy of reducing the ratio of more active but less stable pyrrolic N-coordinated Fe (S1) sites, this study provided an alternative pathway for breaking the activity–stability trade-off of the Fe–N–C catalyst without significantly reducing the ratio of S1 sites.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Research
·
2019
·
IF 0
Ting He,Bingzhang Lu,Yang Chen,Yong Wang,Yaqiang Zhang,John L. Davenport,Alan P. Chen,Chih-Wen Pao,Min Liu,Zhifang Sun,Alexander Stram,Alexander Mordaunt,Jairo Velasco,Yuan Ping,Yi Zhang,Shaowei Chen
Rational design of single-metal atom sites in carbon substrates by a flexible strategy is highly desired for the preparation of high-performance catalysts for metal-air batteries. In this study, biomass hydrogel reactors are utilized as structural templates to prepare carbon aerogels embedded with single iron atoms by controlled pyrolysis. The tortuous and interlaced hydrogel chains lead to the formation of abundant nanowrinkles in the porous carbon aerogels, and single iron atoms are dispersed and stabilized within the defective carbon skeletons. X-ray absorption spectroscopy measurements indicate that the iron centers are mostly involved in the coordination structure of FeN4, with a minor fraction (ca. 1/5) in the form of FeN3C. First-principles calculations show that the FeNx sites in the Stone-Wales configurations induced by the nanowrinkles of the hierarchically porous carbon aerogels show a much lower free energy than the normal counterparts. The resulting iron and nitrogen-codoped carbon aerogels exhibit excellent and reversible oxygen electrocatalytic activity, and can be used as bifunctional cathode catalysts in rechargeable Zn-air batteries, with a performance even better than that based on commercial Pt/C and RuO2 catalysts. Results from this study highlight the significance of structural distortions of the metal sites in carbon matrices in the design and engineering of highly active single-atom catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qisheng Huang,Shaojian Xie,Lei Sheng,Lei Huang,Jia Yan,Zhenxin Chen,Meng Li,Hongguo Zhang
Fluoride pollution is becoming increasingly serious with industrial growth. Controlling fluoride pollution have become important environmental issues of global concern. Transition metal nitrides are excellent CDI electrode materials due to their excellent conductivity and electrochemical stability. In this study, FeN x /C was synthesized as an electrode material for using the capacitive deionization (CDI) technique to achieve the effective removal of fluoride ions from wastewater. Its high specific surface area (463.278 mg/g) and high capacitance (44.29 F/g) were demonstrated and it had a high adsorption capacity of 158.33 mg/g. FeN 3 and FeN 4 were used as the main sites as capacitive deionization for removing fluoride from the water by chemisorption and hydrogen bonding. The higher adsorption energy by density functional calculation also indicated that the existence of Fe-N coordination bond effectively improved its electrosorption capacity. This study is beneficial to provide references and research ideas for removing fluoride in the CDI field.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Jingjing Hu,Sen Wang,Jiaqi Yu,Wenkai Nie,Jie Sun,Shaobin Wang
Heterogeneous electro-Fenton (HEF) reaction has been considered as a promising process for real effluent treatments. However, the design of effective catalysts for simultaneous H2O2 generation and activation to achieve bifunctional catalysis for O2 toward •OH production remains a challenge. Herein, a core–shell structural Fe-based catalyst (FeNC@C), with Fe3C and FeN nanoparticles encapsulated by porous graphitic layers, was synthesized and employed in a HEF system. The FeNC@C catalyst presented a significant performance in degradation of various chlorophenols at various conditions with an extremely low level of leached iron. Electron spin resonance and radical scavenging revealed that •OH was the key reactive species and FeIV would play a role at neutral conditions. Experimental and density function theory calculation revealed the dominated role of Fe3C in H2O2 generation and the positive effect of FeNx sites on H2O2 activation to form •OH. Meanwhile, FeNC@C was proved to be less pH dependence, high stability, and well-recycled materials for practical application in wastewater purification.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhenyu Yan,Wenyu Gao,Chenkai Zhong,Qiangqiang Jiao,Xiuyun Zhao,Jia Liu
Fe-Nx sites can activate peroxymonosulfate (PMS) in advanced oxidation processes (AOPs) to produce various reactive oxygen species, and have great potential for removing tetracycline (TC), but their formation and catalytic mechanism are rarely studied. Herein, the Fe/N-C catalyst was prepared by crosslinking chitosan (CS) using a coordination complex of Fe 2+ and phenanthroline as the precursor for FeNx. The results of crystal structure, lattice constant, chemical state of N element and structural analysis have demonstrated the successful construction of FeNx sites. The degradation experiments confirmed that the removal efficiency of tetracycline reached up to 90.7 % within 15 min, with a degradation rate of up to 0.184 min −1 . Moreover, the material has exhibited excellent performance in complex water environments and within a broad pH range (pH = 2.30 ∼ 9.88). Mechanism analysis proves that the active substances in the system are 1 O 2 , •O 2 − , SO 4 •− , •OH and Fe IV = O, of which 1 O 2 played the principal role. The FeNx structure is the primary active site, where the redox cycle between Fe 2+ and Fe 3+ , electron transport between pyridinic N, electron-deficient C and PMS produces active components. In addition, based on the various intermediate products detected, two possible TC degradation pathways are reasonably speculated. In this study, the highly active FeNx sites were successfully constructed, and elucidated their activation mechanism towards PMS, which proved the broad prospect of Fe/N-C materials in pollutant degradation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Li Gong,Xiaojiang Qiu,Paul G. Tratnyek,Chengshuai Liu,Feng He
FeNX in Fe single-atom catalysts can be the active site for adsorption and activation of reactants. In addition, FeNX species have been shown to facilitate electron transfer between Fe and the carbon supports used in newly developed metal–air batteries. We hypothesized that the combination of FeNX species with granular zero-valent iron (ZVI) might result in catalyzed reductive decontamination of groundwater contaminants such as trichloroethylene (TCE). Here, such materials synthesized by ball milling microscale ZVI with melamine and the resulting N species were mainly in the form of pyridinic, pyrrolic, and graphitic N. This new material (abbreviated as N–C-mZVIbm) dechlorinated TCE at higher rates than bare mZVIbm (about 3.5-fold) due to facilitated electron transfer through (or around) the surface layer of iron oxides by the newly formed Fe–NX(C). N–C-mZVIbm gave higher kTCE (0.4–1.14 day–1) than mZVIbm (0–0.4 day–1) over a wide range of pH values (4–11). Unlike most ZVI systems, kTCE for N–C-mZVIbm increased with increasing pH values. This is because the oxide layer that passivates Fe0 at a high pH is disrupted by Fe–NX(C) formed on N–C-mZVIbm, thereby allowing TCE dechlorination and HER under basic conditions. Serial respike experiments gave no evidence of decreased performance of N–C-mZVIbm, showing that the advantages of this material might remain under field applications.
研究领域:
环境科学
·
材料化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）