LANGMUIR
·
2025
·
IF 3.9
Caiqin Miao,Xinyue Shi,Zhijian Li,Xiaoyong Zhang,Xinzhi Wang,Depeng Yang,Qun Wang
The coexisting anticorrosion and antibacterial functions are of great significance for the marine industry. Controllable surface negative charge and wettability of pyrrolic nitrogen-doped carbon dots (NCDs) derived from the single antibiotic norfloxacin precursor with a special nitrogen heterocyclic structure were successfully fabricated through the hydrothermal route. The incorporated functional groups and chemical bonds, surface charge, mechanism of pyrrole nitrogen ring formation at the molecular level, and antibacterial properties of NCDs were revealed by FTIR, XPS, zeta potential, LC–MS, and electrochemical techniques. The present corrosion efficiency (96.1%) in 3.5 wt % NaCl saline solution in the presence of air and N2 or UO22+ is higher than most previously reported values. The proposed electron transfer corrosion mechanism suggests that the negative charge domains of NCDs were strengthened by the saltwater electron sink effect to repel chlorine and simultaneously a large number of electrons of NCDs were injected into copper as the electron reservoir based on energy-level matching, thereby avoiding Cu0 oxidization. Current works provide a guideline for exploring novel eco-friendly and highly efficient NCD corrosion inhibitor materials with antibacterial properties for safeguarding metals in seawater.
研究领域:
材料科学
·
腐蚀科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Hui Jiang,Lin Liu,Kai Zhao,Zhen Liu,Xinsheng Zhang,Shuozhen Hu
Nitrogen doping was widely used to increase the electronic density of carbon materials and to enhance the adsorption of the supported metal catalysts . However, the exact interaction between various doped nitrogen species and palladium (Pd) have rarely been reported for formic acid electrooxidation (FAO). In this study, the effect of the doped pyridinic-N and pyrrolic-N on the electronic structure and the electrochemical activity of Pd toward FAO are investigated. The oxidation state of Pd is reduced and more metallic Pd is formed when Pd nanoparticles supported on pyridinic-N and pyrrolic-N doped carbon materials . Density functional theory (DFT) calculations simulate that the adsorption energy of HCOO* and *COOH on Pd/pyrrolic-N are lower than those on Pd/pyridinic-N. Both DFT and electrochemical measurements suggest that the FAO activity of Pd is more correlated with the pyrrolic-N than pyridinic-N. The catalyst contains more pyrrolic-N species exhibits higher electrochemical activity and faster kinetics for FAO reaction. Moreover, Pd 2+ -N complexes are formed in all the nitrogen doped catalysts and display good activity for FAO. In this study, Pd supported on urea treated carbon (Pd/UR) owns the highest content of pyrrolic-N and exhibits the best activity for FAO.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Materials
·
2018
·Vol. 11
·期 1
·159
·
IF 2.467
Liqing Li,Xiancheng Ma,Ruofei Chen,Chunhao Wang,Mingming Lu
Nitrogen-doped porous carbon (ZC) is prepared by modification with ammonia for increasing the specific surface area and surface polarity after carbonization of zeolite imidazole framework-8 (ZIF-8). The structure and properties of these ZCs were characterized by Transmission electron microscopy, X-ray diffraction, N2sorption, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. Through static adsorption tests of these carbons, the sample obtained at 600 °C was selected as an excellent adsorbent, which exhibited an excellent acetone capacity of 417.2 mg g−1(25 °C) with a very large surface area and high-level nitrogen doping (13.55%). The microporosity, surface area and N-containing groups of the materials, pyrrolic-N, pyridinic-N, and oxidized-N groups in particular, were found to be the determining factors for acetone adsorption by means of molecular simulation with density functional theory. These findings indicate that N-doped microporous carbon materials are potential promising adsorbents for acetone.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Jun Wan,Guoqun Zhang,Hongrun Jin,Jiabin Wu,Nian Zhang,Bin Yao,Kaisi Liu,Meilin Liu,Tonghuan Liu,Liang Huang
While nitrogen (N)-doped carbon can facilitate the four-electron transfer in oxygen reduction reaction (ORR), its effect on the two-electron path is yet to be investigated. To date, the random N-C bond configurations in N-doped carbons make it difficult to identify the active sites for electrochemical reactions . Here, we report a preparation of well-controlled N-C configurations with high centrality as model catalysts for identification of active sites for two-electron transfer ORR. Specifically, the synthesized Pyrrolic-N doped single-wall carbon nanotube and graphene utilizing a microwave-assisted pulse heating method, exhibit excellent activity for two-electron path (H 2 O 2 selectivity of 93.5% and 98.35%). X-ray adsorption near-edge structure spectroscopy measurements indicate that carbon atoms adjacent to Pyrrolic-N are the active sites for two-electron transfer. This work provides a viable way for the fabrication of tailored N configurations in carbon materials and significantly advances our understanding of the N moieties for the electrochemical H 2 O 2 generation.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-10
·
IF 12.121
Tian Kesong,Wang Junyan,Cao Ling,Yang Wei,Guo Wanchun,Liu Shuhu,Li Wei,Wang Fengyan,Li Xueai,Xu Zhaopeng,Wang Zhenbo,Wang Haiyan,Hou Yanglong
Integrating nitrogen species into sp 2 -hybridized carbon materials has proved an efficient means to improve their electrochemical performance. Nevertheless, an inevitable mixture of nitrogen species in carbon materials, due to the uncontrolled conversion among different nitrogen configurations involved in synthesizing nitrogen-doped carbon materials, largely retards the precise identification of electrochemically active nitrogen configurations for specific reactions. Here, we report the preparation of single pyrrolic N-doped carbon materials (SPNCMs) with a tunable nitrogen content from 0 to 4.22 at.% based on a strategy of low-temperature dehalogenation-induced and subsequent alkaline-activated pyrolysis of 3-halogenated phenol-3-aminophenol-formaldehyde (X-APF) co-condensed resins. Additionally, considering that the pseudocapacitance of SPNCMs is positively dependent on the pyrrolic nitrogen content, it could be inferred that pyrrolic nitrogen species are highly active pseudocapacitive sites for nitrogen-doped carbon materials. This work gives an ideal model for understanding the contribution of pyrrolic nitrogen species in N-doped carbon materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Mingjun Cui,Yujie Qiang,Wei Wang,Haichao Zhao,Siming Ren
In this work, nitrogen doped carbon dots (NCDs) were prepared with citric acid monohydrate (CA·H 2 O) and ethanolamine (EA) via microwave method. In combination with electrochemical techniques, weight loss and SEM, it is found that nitrogen doping in carbon dots effectively suppresses the corrosion of Q235 carbon steel in HCl solution owing to the presence of pyrrolic N in NCDs. Especially for NCDs (1:10), the optimum inhibition efficiency is about 89% after 1 h of immersion in 0.1 M HCl solution with 500 ppm of concentration. By further calculation, the Δ G ads 0 value for NCDs (1:10) is -26.65 kJ·mol -1 , indicating the adsorption of NCDs on Q235 carbon steel surface involves both chemisorption and physisorption. In addition, NCDs still remain superior corrosion inhibition performance with the prolonged immersion time and ascending temperature.
研究领域:
材料科学
·
腐蚀与防护
·
电化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Huirong Zhang,Yi Shen,Xiaokai Shi,Jinlei Cui,Baofeng Wang,Yanxia Guo,Dongke Zhang,Fangqin Cheng
Persistent environmental pollution by heavy metals, particularly Cr (VI), poses significant risks to ecosystems and human health due to its high toxicity and bioaccumulation potential. The development of high-performance, cost-effective adsorbents from sustainable materials remains a critical challenge in the field of Cr (VI) remediation. This study investigates the influence of pyrrolic-N (N-5) within nitrogen-doped hierarchical porous carbon (N-HPC) on its adsorption capacity. Results indicate that N-HPC variants with a higher N-5 content exhibit superior adsorption abilities. The optimal sample demonstrated an exceptional adsorption capacity of 386.2 mg/g for Cr (VI). Even after seven regeneration cycles, this N-HPC variant maintained a remarkable 77.8 % removal efficiency for Cr (VI), highlighting its robust stability and selectivity. The relationship between the physicochemical properties of N-5 and N-HPC was thoroughly examined, revealing that N-5 plays a crucial role in the adsorption process. Due to its high electronegativity, nitrogen-doping into the carbon framework generates a dipole moment, enhancing the electronegativity of N-HPC, altering its local electron density and polarity, increasing specific surface area, carbon defect density, and ion exchange capacity. These factors collectively contribute to significant improvements in pore filling, ion exchange efficiency, and electrostatic adsorption by N-HPC. The reduction complexation mechanism emerges as the dominant factor in the adsorption process. N-5 not only provides reducing electrons as an electron donor, facilitating the continuous conversion of Cr (VI) to Cr (III), but also acts as an adsorption active site, complexing Cr to the surface of N-HPC. This synergistic effect strengthens the reduction complexation, enhances adsorption performance, and improves the regeneration cycle and adsorption selectivity for Cr.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shixuan Zhu,Dexu Zhang,Zhihong Xue,Yiqiang He,Cailing Chen,Zhan Shi
Establishing robust atomic-level interfaces, particularly through the selective modulation of surface active sites within heterojunctions to achieve superior solar energy conversion, remains largely unexplored. Herein, sulfur vacancy sites (V S ) in ZnIn 2 S 4 (ZIS) are selected, driven by the interaction between unsaturated zinc sites and the nitrogen-rich sites of g-C 3 N 4 , forming a step-scheme (S-scheme) heterojunction. The defect-induced interfacial Zn–N–C bonds not only provide rapid channels at the atomic level, thereby lowering the energy barrier for charge transfer, but also selectively tune the highly active pyrrolic N site to enhance H 2 evolution. Furthermore, molecular dynamics simulations (MD) combined with density functional theory (DFT) calculations reveal that V S regulates the pyrrolic N sites within the heterojunction, leading to a reduction in the Gibbs free energy for hydrogen production. Kinetic analysis by carrier transport activation energy (CTAE) indicates that the charge transfer energy barrier is accelerated, decreasing from 211.20 eV for ZIS/CN-360 % to 155.71 eV for V S -ZIS/CN-360 %. Consequently, the designed catalyst significantly enhances the H 2 yield (27.94 mmol g −1 h −1 ) in the absence of platinum. This work emphasizes the importance of generating defect-induced interfacial atomic channels, as well as changes in the surface microenvironment, which underscore the significance of defect heterostructures in promoting the photocatalytic process.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 24
·19665-19670
·
IF 3.201
Xiangyu Lu,Dan Wang,Liping Ge,Lihui Xiao,Haiyan Zhang,Lilai Liu,Jinqiu Zhang,Maozhong An,Peixia Yang
Nitrogen-doped graphene (N-G) is considered as a promising catalyst for the oxygen reduction reaction (ORR). However, the contributions of pyridinic N, pyrrolic N and graphitic N in N-G for the ORR catalytic activity are controversial. In this work, the contents of pyridinic N, pyrrolic N and graphitic N in N-G were transformed by annealing at different temperatures. It is found that the total N content in N-G is not the critical factor to determine the ORR activity. An increase in the annealing temperature can enhance the content of graphitic N in N-G, causing an improved catalytic ORR activity, which confirms that graphitic N is the active component. Moreover, the enriched graphitic N in the N-G-1000 catalyst shows a half-wave potential (E1/2) of 0.862 V, 29 mV higher than that of the commercial Pt/C catalyst (0.833 V), which is one of the best reported for ORR metal-free catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Menglei Yuan,Lei Zhang,Tianxin Wang,Yiming Liu,Qiongguang Li,Jinxiong Wu,Junwu Chen,Jintong Zhang,Hailun Yang,Guangjin Zhang
Electrocatalytic water splitting in an alkaline medium is recognized as the promising technology to sustainably generate clean hydrogen energy via hydrogen evolution reaction (HER), while the sluggish water dissociation and subsequent *H adsorption steps greatly retarded the reaction kinetics and efficiency of the overall hydrogen evolution process. Whilst nitrogen (N)-doped carbon-based materials are attractive candidates for promoting HER activity, the facile fabrication and gaining a deeper insight into the electrocatalytic mechanism are still challenging. Herein, inspired by the Diels-Alder reaction, we precisely tailored six-membered pyridinic N and five-membered pyrrolic N sites at the edge of the carbon substrates. Comprehensive analysis validates that the participation of pyridinic N (electron-withdrawing) and pyrrolic N (electron-releasing) will induce the charge rearrangements, and further generate local electrophilic and nucleophilic domains in adjacent carbon rings, which guarantees the occurrence of water dissociation to generate protons and the subsequent adsorption of *H intermediates through electrostatic interactions, thereby facilitating the overall reaction kinetics. To this end, the optimal NC-ZnCl 2 -25 % electrocatalysts present excellent alkaline HER activity (η 10 = 45 mV, Tafel slop of 37.7 mV dec -1 ) superior to commercial Pt/C.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers of Materials Science
·
2023
·Vol. 17
·期 4
·1-12
·
IF 2.7
Liu Fangfang,Niu Jinan,Chuan Xiuyun,Zhao Yupeng
Nitrogen atom doping has been found to enhance the electrochemical performance of porous carbon (PC). In this study, hollow tubular nitrogen-doped porous carbon (N/PC) was synthesized using polyvinylpyrrolidone as the carbon–nitrogen source and fibrous brucite as the template through carbonization. The effects of nitrogen and argon protective atmospheres on the nitrogen content, the specific surface area (SSA), and electrochemical properties of N/PC were investigated. The results showed that compared with N/FBC-Ar, N/FBC-N 2 prepared in nitrogen protective atmosphere had a higher nitrogen content and a larger proportion of pyrrolic nitrogen (N-5) and pyridinic nitrogen (N-6). N/FBC-N 2 displayed a specific capacitance ( C ) of 194.1 F·g −1 at 1 A·g −1 , greater than that of N/FBC-Ar (174.3 F·g −1 ). This work reveals that the nitrogen doping with a higher nitrogen content in nitrogen protective atmosphere is more favorable. Furthermore, a larger proportion of pyrrolic nitrogen and pyridinic nitrogen in the doped nitrogen atoms significantly enhances the electrochemical performance.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Zeyang Chen,Xin Weng,Qibin Zeng,Yunhe Xie,Yifan Liu,Yuancai Lv,Minghua Liu
Nitrogen-doped porous carbon materials derived from agricultural waste are considered ideal for supercapacitor applications. However, current research is limited to nitrogen doping, with insufficient analysis of the effects of different nitrogen species on capacitor performance. This study compares four different nitrogen sources, revealing that the MN-AC electrode material, prepared using melamine as the nitrogen source, effectively enhances the physicochemical structure and electrochemical performance of the electrode. It exhibits the highest surface nitrogen content (4.54 %) and an optimal mesopore rate (20.6 %), with a significant amount of pyrrole nitrogen (53.19 % of the surface content), which notably improves the material's polarization and wettability, thereby enhancing its electrochemical performance. At a current density of 0.5 A g −1 , MN-AC demonstrates a high specific capacitance of 349.3 F g −1 . Furthermore, in a 6 M KOH electrolyte, it achieves an energy density of 20.3 Wh kg −1 and a power density of 169 W kg −1 . DFT analysis indicates that pyrrole nitrogen increases the material's dipole moment, enhancing the adsorption of electrolyte ions (K + ).
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）