CARBON
·
2025
·
IF 11.6
Lianzhong Shen,Lin Wang,Zhouwei Li,Yu Ye,Qizhou Dai
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts are one of the more popular materials for electrochemical reduction of CO 2 to fuels and chemicals. Still, their Faraday efficiency and current density are generally low due to the single coordination environment and defect sites. Heteroatom doping has been demonstrated to increase the degree of defects in the material, improve the electron distribution at the single atomic sites, and enhance the catalytic performance. In this study, we prepared an S-doped single-atom catalyst called FeS@PC by a simple high-temperature pyrolysis method for efficient electroreduction of CO 2 to CO, with a maximum CO Faraday efficiency of 97.0% at -0.6 V vs. RHE potential. S atoms doped in the second-shell can change the electron distribution on the Fe-N 4 sites and accelerate the electron transfer during the electrochemical CO 2 reduction reaction (CO 2 RR). Through in situ ATR-FTIR characterization and kinetic experiments, it is found that the doped S can also promote the dissociation of H 2 O, provide sufficient protons for the conversion of CO 2 to *COOH, and promote the rate of CO conversion.
研究领域:
材料科学
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催化化学
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Ziyi Wang,Xin Lian,Rongyan Yang,Xiaomeng Guo,Shengjie Wei,Jijie Zhang,Xian-He Bu
Introducing polarity in traditional metal-N4 catalytic sites and strengthening the adsorption of polar NO2* intermediate are advantageous for the deep reduction of nitrate into ammonia. Herein, the planar chlorination engineering strategy successfully introduced the C–Cl bonds adjacent to the Fe–N4 catalytic site with higher polarity, effectively boosting the catalytic activity for the nitrate reduction reaction (NO3RR). The maximal NH3 yield rate and the corresponding turnover frequency (TOF) value catalyzed by the Fe–N4/CNCl catalyst were 1.82 mg h–1 cm–2 and 245 h–1 at −0.83 V vs RHE, which were 3.4 times and 2.7 times those of the traditional Fe–N4/CN catalyst without polarity, respectively. The Fe–N4/CNCl catalyst also exhibited satisfactory stability during consecutive 15 cycles. The density functional theory (DFT) calculation revealed that the planar chlorination engineering of the Fe–N4 site with higher polarity strengthened the adsorption of polar NO2* intermediate, facilitated the deep reduction of nitrate into ammonia, lowered the energy barrier of rate-determining step (RDS) and thus improved the catalytic activity. This work exhibited the enormous advantage of a planar chlorination engineering strategy for enhancing the activity of electrocatalysis by introducing polarity in the traditional metal-N4 catalytic site.
研究领域:
材料科学
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电催化
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 23
·13678-13687
·
IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Xiangyu Lu,Jingyuan Ma,Ruopeng Li,Lihui Xiao,Jinqiu Zhang,Maozhong An
Compared to individual metal sites, e.g. Fe–N4 sites, the synergistic effect of dual-metal sites can further adjust the interaction of reactants or intermediates with active sites, which is beneficial for boosting the oxygen reduction reaction (ORR) in Zn–air batteries. However, developing a simple and direct method instead of complicated procedures and post-treatment to realize well-defined dual-metal sites is still a grand challenge. Herein, a facile one-step impregnation-pyrolysis route without any post-treatment is developed to controllably synthesize Fe and Co dual-metal sites embedded in hierarchical N-doped carbon from metal–organic frameworks. X-ray absorption spectra coupled with density functional theory calculations demonstrate that the Fe–N4 and Co–N4 dual sites can synergistically enhance the ORR activity. Impressively, the well-controlled FeCo–N–C catalyst exhibits excellent ORR performance, with half-wave potentials (E1/2) of 0.807 and 0.904 V in 0.1 M HClO4 and 0.1 M KOH, respectively. Benefiting from the highly active dual-metal sites and desired porous structure, FeCo–N–C serving as a cathode catalyst achieves an uplifting peak power density of 196.3 mW cm−2 and a remarkable specific capacity of 728.6 mA h gZn−1 at a discharge current density of 20 mA cm−2 in a practical liquid Zn–air battery. Besides this, such superb battery performance is demonstrated in an all-solid-state Zn–air battery.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 8
·2079-2084
·
IF 8.183
Wang Hong-Hui,Lv Li-Bing,Zhang Shi-Nan,Su Hui,Zhai Guang-Yao,Lei Wei-Wei,Li Xin-Hao,Chen Jie-Sheng
The rational design of highly active and stable atomically dispersed M-X 4 (M = Fe, Co, Ni, etc., X = C, N) -based catalysts holds promises for wide application in almost all realms of catalysis. Despite great effort in the construction of specific M-X 4 centers, the possible effect of non-coordinated heteroatoms on the catalytic activity of metal centers has been rarely explored. Herein, we develop a new type of M-X 4 catalyst composed of Fe-N 4 centers and non-coordinated B heteroatoms (FeNC+B) and find the key role of non-coordinated B adjacent to Fe-N 4 centers in tailoring their electron density and final catalytic selectivity. The experimental and theoretical results demonstrated that non-coordinated boron atoms could decrease the electron density of Fe-N 4 centers to a suitable level and thus boost the selective production of nitriles from amine oxidation by depressing the formation of imines due to the flattened energy barrier of the reversible conversion of imines back to amines. As a reusable heterocatalyst, the state-of-the-art FeNC+B catalyst provides a turn-over frequency (TOF) value of 21.6 mol benzonitrile ·mol Fe −1 ·h −1 (100 °C), outpacing that of bench-marked nonnoble-metal-based homogeneous catalyst by a factor of 3.4.
研究领域:
催化化学
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材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fengliang Cao,Qingshan Zhao,Debin Kong,Xiaojie Tan,Xinxin Li,Tengfei Liu,Linjie Zhi,Mingbo Wu
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts show great potential for heterogeneous catalysis. However, recognizing and engineering the microenvironment of M-N x sites to achieve satisfactory catalytic performance remains challenging. Herein, we propose a facile g-C 3 N 4 -assisted template strategy to anchor atomic Fe-N 4 sites on highly nitrogen-doped carbon nanosheets. Through regulating the ratio and type of peripheral nitrogen species by carbonization temperature, the optimal Fe-N-C-800 catalyst showed significantly boosted catalytic activities (overall turnover frequency of 13.43 min −1 and activation energy of 19.44 kJ mol −1 ) for nitroarene reduction with extremely low reductant dosage, exceeding most reported metal catalysts. Experimental and theoretical results reveal appropriate graphitic- and pyrrolic-N dopants surrounding the Fe-N 4 center can tailor the local electronic structure and contribute to obvious upshift of the d-band center, which dramatically promotes the adsorption and conversion of reactant substrates, eventually delivering the unprecedented catalytic performance. This work provides a guide for rational coordination environment regulation of single-atom catalysts for efficient chemical transformations.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Chen Tiantian,Zhang Ganbing,Sun Hongwei,Hua Yetong,Yang Shu,Zhou Dandan,Di Haoxin,Xiong Yiling,Hou Shenghuai,Xu Hui,Zhang Lizhi
The microenvironment regulation of Fe-N 4 single atom catalysts (SACs) critically governs peroxymonosulfate (PMS) activation. Although conventional heteroatom substitution in primary coordination enhances activity, it disrupts Fe-N 4 symmetry and compromises stability. Herein, we propose oxygen doping in the secondary coordination shell to construct Fe-N 4 -C 6 O 2 SAC, which amplifies the localized electric field while preserving the pristine coordination symmetry, thus trading off its activity and stability. This approach suppresses Fe-N bond structural deformation (bond amplitude reduced from 0.875–3.175 Å to 0.925–2.975 Å) during PMS activation by lowering Fe center electron density to strengthen Fe-N bond, achieving extended catalytic durability (>240 h). Simultaneously, the weakened coordination field lowers the Fe=O σ* orbital energy, promoting electrophilic σ-attack of high-valent iron-oxo towards bisphenol A, and increasing its degradation rate by 41.6-fold. This work demonstrates secondary coordination engineering as a viable strategy to resolve the activity-stability trade-off in SAC design, offering promising perspectives for developing environmental catalysts.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhengwen Fan,Xinjiao Cui,Jiankun Wei,Chan Chen,Haolin Tang,Junsheng Li
Fe N C is the most promising material to replace the noble metal catalyst for cathodic oxygen reduction reaction in proton exchange membrane fuel cells (PEMFCs). However, the practical performance of Fe N C catalyst is significantly limited by its low active site (Fe-N 4 ) density. Herein, we propose to promote the formation of Fe-N 4 active sites in Fe N C catalyst by strengthening the interaction of N precursors and Fe precursors during the carbonization synthesis. In our approach, ionic liquid (IL, [EMIM][NTf 2 ]) with high nitrogen content and good thermal stability is caged in the pores of Fe-ZIF-8 through the host–guest interactions. These interactions are critical for the preservation of Fe and N species and formation of active sites during the synthesis. The optimal catalyst developed with this approach (Fe 0.05 N C/10) has a high density of accessible Fe-N 4 sites (1.88*10 19 sites g −1 ). Therefore, in both acidic and alkaline media, Fe 0.05 N C/10 showed excellent ORR activity comparable to commercial Pt/C catalyst. Moreover, PEMFC performance with a peak power density of 300 mW cm −2 was demonstrated with Fe 0.05 N C/10 under H 2 /O 2 conditions. The synthetic approach reported herein may be used for tailoring of advanced catalyst with high intrinsic activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1232-1238
·
IF 2.726
Chen Weijie,Xia Huicong,Guo Kai,Jin Wangzhe,Du Yu,Yan Wenfu,Qu Gan,Zhang Jianan
Lithium-sulfur(Li-S) batteries have been puzzled by the “shuttle effect”. In the recent years, catalytic materials present a huge potential for solving this problem. However, the exploitation for catalytic activity was still challenging in Li-S batteries. In this article, we put forward a single atom catalyst (SAC) of FeN 4 coupled with Fe 3 C on the N-doped carbon (FeN 4 /Fe 3 C@NC) by one-step pyrolysis method. The FeN 4 and Fe 3 C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in Li-S batteries. As a result, the FeN 4 /Fe 3 C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g). In addition, the FeN 4 /Fe 3 C@NC maintains 99.01% of the pristine specific capacity after 100 cycles at 0.5 C, indicating the improved electrochemical performance in Li-S batteries. This work sheds new lights on the design of engineering catalysts for developing high-performance Li-S batteries.
研究领域:
电化学
·
能源材料
·
纳米催化
·
电池技术
·
材料化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Meiling Fan,Peipei Liu,Yapeng Cheng,Haolin Tang,Bing Jin,Haining Zhang
Design and synthesis of earth-abundant elements-based electrocatalysts with sufficient activity and stability remain challenging for oxygen-involved electrochemical energy conversion and storage devices. In this work, catalyst with simultaneously engineered Fe-N 4 and Co-N 4 active sites and graphitic carbon multilayer-encapsulated FeCo alloy is developed by pyrolysis of metal salts doped G-g-C 3 N 4 . The obtained composite material exhibits promising catalytic activity and good stability for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline electrolyte , as evidenced by the positive shift of half-wave potential by 44 mV compared to 20% Pt/C for ORR and the potential of 1.596 V at current density of 10 mAcm −2 for OER. In addition, the thus-assembled rechargeable zinc-air battery using the synthesized material as cathode delivers a maximum power density of 311.2 mWcm −2 with an open circuit potential of 1.51 V and a long-term cycling stability. DFT calculation results indicate that catalyst with composite active sites displays smaller energy barrier than that with single active site.
研究领域:
材料科学
·
电化学能源
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Shuling Liu,Tongjun Li,Guozheng Dong,Xinao Wei,Keke Zhao,Bangan Lu,Yu Chen,Yanyan Liu,Jianchun Jiang,Baojun Li
To develop low-cost and efficient oxygen reduction reaction (ORR) electrocatalysts, single-atom catalysts (SACs) have attracted great attention to become vital to the applications of zinc-air batteries (ZABs) because of their high catalytic activity. The development of integrated SACs as self-supporting electrodes is crucial for ZABs to overcome the drawback of powder catalysts requiring binder. Herein, an integrated atomically dispersed FeSA/NC catalyst was obtained by pyrolysis of Fe-containing ZIF-8 on fir wood-derived carbon. The atomically dispersed Fe-N4 is an efficient catalytic active site for ORR. The self-supported ordered porous structure and continuous conductive network of the catalyst provide favorable conditions for the rapid mass/electron transfer. FeSA/NC catalyst demonstrates a positive half-wave potential of 0.90 V in 0.1 M KOH electrolyte and 0.80 V in acidic solution. The outstanding ORR activity outperforms those of commercial Pt/C and most reported M-N-C (M=Fe, Co, Ni, etc.) catalysts. A quasi-solid-state ZAB using the FeSA/NC in cathode shows an excellent peak power density of 77 mW cm–2 at 121 mA cm–2. The performance in quasi-solid-state batteries exceeds that of most other catalysts. This work provides a new path to the catalytically active carbon via design of self-supporting SACs, and a clear demonstration of prospects in quasi-solid-state energy devices.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Lihui Xiao,Yaqiang Li,Peixia Yang,Qiang Lv,Xiangyu Lu,Hao Xu,Ruopeng Li,Huiling Zhang,Shengbo Yang,Anmin Liu,Dan Wang,Jinqiu Zhang,Maozhong An
Carbon nanotubes' (CNTs) preparation and formation mechanisms are of great interest. To improve their performance in the oxygen reduction reaction (ORR), a post-treatment to add active centers is required. This study presents a simple method using a molten-salt template to self-assemble bamboo-shaped CNTs (B-Fe-N-C) with highly stable Fe-N 4 (Fe-pyridinic-N 4 ) sites. By analyzing the evolution of high-temperature materials and the intermolecular bonding process, the formation mechanism of B-Fe-N-C follows a two-dimensional material synthesis--bonding--self-assembly--growth mechanism. Impressively, B-Fe-N-C exhibits superior ORR performance (a half-wave potential of 0.868 V) and stability (only 3 mV attenuation after 10000 cycles of accelerated durability test) in alkaline medium. Density functional theory calculations demonstrate that Fe-Pyridinic-N 4 sites can lower the energy barrier for ORR. Furthermore, Comsol multiphysics simulations confirm the significant enhancement of oxygen mass transfer by bamboo-shaped B-Fe-N-C. Therefore, B-Fe-N-C is employed in zinc-air batteries, resulting in nice discharge performance and high peak power density.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Bai Jingsen,Zhao Tuo,Xu Mingjun,Mei Bingbao,Yang Liting,Shi Zhaoping,Zhu Siyuan,Wang Ying,Jiang Zheng,Zhao Jin,Ge Junjie,Xiao Meiling,Liu Changpeng,Xing Wei
The limited durability of metal-nitrogen-carbon electrocatalysts severely restricts their applicability for the oxygen reduction reaction in proton exchange membrane fuel cells. In this study, we employ the chemical vapor modification method to alter the configuration of active sites from FeN 4 to the stable monosymmetric FeN 2 +N’ 2 , along with enhancing the degree of graphitization in the carbon substrate. This improvement effectively addresses the challenges associated with Fe active center leaching caused by N-group protonation and free radicals attack due to the 2-electron oxygen reduction reaction. The electrocatalyst with neoteric active site exhibited excellent durability. During accelerated aging test, the electrocatalyst exhibited negligible decline in its half-wave potential even after undergoing 200,000 potential cycles. Furthermore, when subjected to operational conditions representative of fuel cell systems, the electrocatalyst displayed remarkable durability, sustaining stable performance for a duration exceeding 248 h. The significant improvement in durability provides highly valuable insights for the practical application of metal-nitrogen-carbon electrocatalysts.
研究领域:
材料科学
·
电化学
·
能源工程
✓ 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）