Journal of Materials Chemistry A
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2021
·Vol. 9
·期 23
·13678-13687
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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
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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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
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电化学能源
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Longjian Li,Junhui Wang,Qinhua Zhang,Shuai Wang,Hangkai Zhang,Tao Xing,Mingqing Wang,Mingbo Wu,Zhenxing Wang,Wenting Wu
Near-infrared light occupies 54.3% of the solar spectrum and has greater penetration depth, and its effective utilization is of great significance in the practical application of photocatalysis on a larger scale. However, the development of catalysts that can directly utilize near-infrared light is still a huge challenge. This paper proposes a strategy to directly utilize near-infrared light (excitation wavelength extending to 850 nm) by creating carbon material doped with a high-spin-state Co(II)-Nx single-atom site. In the near-infrared-light-irradiated photooxidation of 1,5-dihydroxynaphthalene, the yield of juglone can reach 45% without a significant decrease, even when the catalytic volume is increased by 20 times, which was much higher than that irradiated by 460 nm wavelength (reduced by about 23%). Our study sets the stage for fabricating stable NIR photocatalysts and provides a solution to directly enhance NIR photooxidation in a large-scale manner.
研究领域:
材料科学
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光化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Tao Ai,Mingling Yu,Yicheng Dai,Ruipu Yao,Ling N. Jin,Yuanyuan Yu,Xinbin Qiu,Peixin Huang,Xifen Zhu,Jianteng Sun,Lizhong Zhu
This study investigates the uptake, biotransformation, and phytotoxicity of sulfadiazine (SDZ) and its acetyl derivative N4-acetylsulfadiazine (NASDZ) in rice. Results showed that rice was more tolerant to NASDZ, with lower malondialdehyde and reactive oxygen species levels but higher antioxidant enzyme activities (SOD, POD, and CAT). The maximum accumulations of SDZ in roots and shoots were 19.3 ± 1.0 and 3.6 ± 1.1 μg/g, while NASDZ were 18.6 ± 2.5 and 3.5 ± 1.4 μg/g, respectively. SDZ exposure generated more metabolic intermediates, including deamination, hydroxylation, glycosylation, acetylation, and formylation products, while NASDZ metabolism was documented for the first time. Key genes involved in biotransformation include cytochrome P450, acetyltransferase, glycosyltransferases, and methyltransferase. Density functional theory calculations showed structural differences affecting reactive sites and intermediates. SDZ disrupted lipid metabolism, while NASDZ altered carbohydrate and amino acid pathways, highlighting their selective effects on rice metabolism. Our data help understand sulfonamide biotransformation and phytotoxicity in rice.
研究领域:
环境科学
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植物生理学
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毒理学
✓ 已验证
DOI
PubMed
高影响因子
CARBON
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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
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Huiyuan Cheng,Xuemei Wu,Xiangcun Li,Xiaowa Nie,Shuai Fan,Manman Feng,Zihao Fan,Mingqian Tan,Yonggang Chen,Gaohong He
Although considerable progress has been achieved by Cu nanoparticles for catalyzing CO 2 reduction reaction (CO2RR), Cu single atom catalysts (Cu SACs) are generally suffered from inferior performance to that of widely investigated Fe, Co, Ni SACs. This phenomenon mainly ascribes to the lack of effective geometry and electronic engineering of copper active center from an atomic level. Herein, highly exposed atomically dispersed Cu-N x ( x denotes Cu–N coordination number) sites anchored on 3D porous carbon matrix are successfully synthesized through facile one step thermal activation, and Cu-N 4 sites exhibit boosted activity and selectivity compared to its nearly inert Cu-N 3 counterparts. Aided by density functional theory (DFT) calculations, the edge-hosted Cu-N 4 moieties are revealed as key active sites for efficient CO generation via optimized local coordination environment and electronic properties, which strongly interact with *COOH intermediate and facilitate the desorption of *CO. As a result, Cu-N 4 catalyst achieves high CO Faradaic efficiency (FE CO ) of over 90% from −0.6 to −1.1 V vs . RHE with a maximum value of 98%, surpassing the previously reported Cu SACs for CO 2 -to-CO conversion. This work provides new insight into proper Cu SACs design and fundamental mechanism understanding to boost CO2RR.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
·
IF 19
Huajie Zhong,Junhui Wang,Bin Zhang,Yangyang Liu,Zeyu Gong,Xinzhe Xiao,Jiaxing Yu,Yu Hou,Yuan Tao,Huangsheng Yang,Qi Fu,Jiating Zheng,Pengfei Wang,Gangfeng Ouyang
Carbon-supported single-atom catalysts (CS-SACs) have attracted tremendous attention in environmental remediation fields, however, the role of the ubiquitously existing carbon defects on the support in regulating the electronic structure of active metal sites has long been overlooked. Herein, a selective pyridinic N etching strategy is proposed to controllably fabricate specific pentagon defects in the carbon supports anchored with Co-N 4 sites. Theoretical and experimental results reveal that the pentagon defects can induce upward shifting of the Co d-band center and increase the electron density in the dxz and dz 2 orbitals, indicating its indispensable role in regulating the electronic structure of the metal center. As a result, efficient electron transfer is realized between the Co atom and peroxymonsulfate (PMS). Moreover, the energy barriers for crucial oxygen intermediate are reduced, which facilitates the generation of singlet oxygen ( 1 O 2 ). Consequently, the Co-N 4 catalyst with pentagon defects (C5-Co-N 4 ) achieved a remarkable TOF value (9.37 min −1 ) in a Fenton-like reaction, surpassing the state-of-the-art single-atom catalysts reported so far. This work not only provides a strategy to controllably fabricate specific defects in CS-SACs but also deepens the fundamental understanding on how pentagon defects regulate the electron structure and catalytic performance of metal-N 4 sites.
研究领域:
环境科学
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催化化学
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材料科学
✓ 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
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
Clinics
·
2025
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IF 2.4
Shan Xu,Xuming Lin,Fengling Jia
Objective Retinoblastoma (RB) is a type of intraocular tumor in childhood with a high lethality rate. N4-acetylcytosine (ac 4 C) modification is known to regulate multiple cancers, which is mediated by the only known ac 4 C writer N-Acetyltransferase 10 (NAT10). In this study, the authors aimed to reveal the mechanism of RB progression regulated by ac 4 C modification. Method Phenotypically, dot blot assay and quantitative real-time PCR were used to detect the ac 4 C levels and NAT10 expression in clinical samples and RB cell lines. Then, NAT10 was knocked down to assess its effect on glycolysis. Mechanically, RNA immunoprecipitation assay, immunofluorescence assay, and dual luciferase report were used to explore the mRNA modified by NAT10-mediated ac 4 C modification. Mice xenograft model was used to determine the effect of NAT10 on tumor growth in vivo . Results The present results demonstrated that the levels of ac 4 C and NAT10 were increased in cancer tissues and RB cell lines. Furthermore, NAT10 knockdown inhibited the glycolysis in RB cell lines. Moreover, the authors revealed that NAT10 knockdown decreased the ac 4 C modification and mRNA stability of HK1, while the inhibition of glycolysis by NAT10 knockdown was reversed by HK1 overexpression. Finally, NAT10 knockdown relieved the growth of tumors in mice models. Conclusion The authors illustrated that NAT10 plays an important role in the progression of RB by regulating the ac 4 C modification on HK1 mRNA and affects its stability, which may provide a novel theoretical basis for the treatment of RB.
研究领域:
肿瘤学
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分子生物学
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医学遗传学
✓ 已验证
产品关联
DOI
PubMed
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
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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
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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
危险品化学品经营许可证（带存储）