Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Li Jiabao,Wang Ruoxing,Han Lanlan,Wang Tianyi,Asakura Yusuke,Wang Chengyin,Wang Guoxiu,Xu Xingtao,Yamauchi Yusuke
Nitrogen-doped carbons (NCs) have demonstrated notable advantages for application in capacitive deionization (CDI). However, the potential roles of different nitrogen configurations in the CDI process, especially how the neglected oxygen doping synergistically works, remain unclear. In this work, we systematically addressed these critical issues and revealed the significant role of trace oxygen doping in enhancing the desalination performance of NC electrodes. By introducing oxygen into nitrogen-doped carbon nanosheets (ONC-S), using guanine as the precursor, we obtained abundant pyridinic and pyrrolic nitrogen configurations. This design aims to synergistically enhance the charge distribution, wettability, and ion diffusion of the target electrodes. Compared with commercial activated carbon and other state-of-the-art materials, our ONC-S electrode demonstrates superior specific capacitance, excellent cycling stability, and enhanced desalination efficiency. These findings highlight the synergistic effects of trace oxygen doping and the nitrogen configuration, offering valuable insights into the mechanisms driving the improved CDI performance.
研究领域:
材料科学
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环境工程
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jun Shi,Xiaoshan Zhang,Sabarinathan Ravichandran,Shirong Sun,Yulong Li,Ruoyu Wu,Wanxuan Luo,Hongmei Xing,Wenli Zhang
We report here the synthesis of N-doped porous carbon (PC) through a convenient melamine pre-grafting strategy. The melamine derivative with a monolayer structure was first grafted on the surface of the micropores of PC using a suitable diazotization reaction of melamine in an aqueous solution. After pyrolysis , PC grafting with melamine derivative was converted to the obtained N-doped PC. Meanwhile, more nitrogen dopants were grafted, and nitrogen functionalities were reconstructed to generate more graphitic N and pyridinic N atoms, in which the mesopores volume was consequently enlarged. Because of the unique structures mentioned above, the as-obtained N-doped PC exhibited enhanced oxygen reduction activity under alkaline compared with the N-doped PC from the standard physical mixture of PC and melamine. Besides, the obtained N-doped PC showed a comparable half-wave potential, remarkable durability, and good methanol tolerance compared with the commercial 20% Pt/C electrocatalyst . The results presented here could guide the development of new and improving metal-free nitrogen-doped porous carbon catalysts toward oxygen reduction reaction.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhao Sun,Ke Li,Sam Toan,Rongjun Zhang,Hongwei Li,Yu Wu,Zhiqiang Sun
Redox nitrogen fixation-nitride hydrolysis looping provides a promising pathway for ammonia synthesis; however, high N fixation temperature and low N 3− lattice supplement efficiency limit its further development and application. In this regard, a two-step chemical looping ammonia synthesis route, chromium-based nitrogen carrier enabled low-temperature N fixation and nitrogen carrier hydrolysis, is proposed to intensify ammonia generation. In the N fixation step, the effects of carbon species on the carbothermal reduction performance are investigated. Results reveal that decreasing the graphitization degree of the carbon species can effectively reduce the nitrogen activation temperature from 1054 °C to 948 °C. Meanwhile, the C/Cr 2 O 3 ratio required is correlated with the amount of oxygen in carbon species, and the appropriate active carbon/biochar-to-Cr ratios are 4.00 and 3.25, respectively. In the ammonia synthesis step, the nitrogen carrier hydrolysis rate is mainly limited by the diffusion of reactive species. The ammonia formation rate reaches 0.127 mmol·h −1 ·g −1 nitrogen carrier at 1100 °C. XRD retrieve refinement results reveal that the utilization of the lattice nitrogen decreases with the increase in the ammonia releasing temperature. This study provides new implications for advanced nitrogen carrier exploitation, which will substantially promote the development of chemical looping ammonia synthesis technologies with lowered energy consumption.
研究领域:
化学工程
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催化
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Weishi Huang,Chenxi Wu,Minghao Gou,Xiaochun Wu,Le Zhang,Ting Liu,Jianlong Wang
The conversion of nitrate nitrogen (NO 3 − -N) or ammonia nitrogen (NH 4 + -N) to dinitrogen (N 2 ) by chemical process for total nitrogen (TN) removal is meaningful, but still a challenge in wastewater treatment. Herein, zero valent iron (Fe 0 ) loaded active carbon (Fe 0 @AC) was prepared and used to remove TN from the nitrogen-containing wastewater by an efficient chemical reduction coupled with oxidation process (FeR-PSO). In the step of NO 3 − -N reduction by Fe 0 @AC, Fe 0 @AC with 25 wt% Fe 0 could reduce 100 % NO 3 − -N with the initial concentration of 50 mg N/L after 60 min at the Fe 0 @AC dosage of 9 g/L and initial pH of 3.0, and over 30 % NO 3 − -N could be reduced to N 2 . In the subsequent oxidation step, persulfate (PS) and magnesium oxide (MgO) were introduced into the solution after NO 3 − -N reduction to selectively oxidize NH 4 + -N to N 2 . The removal efficiency of NH 4 + -N and N 2 selectivity after 30 min were 100 % and over 90 %, respectively, at the MgO dosage of 8 g/L and the PS dosage of 20.25 g/L. The developed FeR-PSO process could remove 93.40 % of TN from simulated wastewater, and over 90 % of TN from two actual pickle factory wastewaters. The possible mechanisms of NO 3 − -N reduction and NH 4 + -N oxidation by FeR-PSO process were proposed. These findings provide new insights for TN removal from NO 3 − -N containing wastewater or wastewater containing both NO 3 − -N and NH 4 + -N by chemical process.
研究领域:
环境科学
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污水处理
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Huimin Shi,Hang Zhang,Zhi Chen,Tao Wang,Lei Wang,Wei Zeng,Guanhua Zhang,Huigao Duan
Titanium nitride (TiN) has been attracting increasing interest as an anode material for electrochemical energy storage and conversion systems due to its superior thermal stability, electrical conductivity and chemical durability. The most commonly used strategy to synthesize TiN nanostructures is nitriding TiO 2 nanostructures using ammonia gas as the nitrogen source, and thus is not environmental friendly. Herein, we report an ammonia-free strategy to synthesize TiN nanomaterials using TiO 2 precursors via a magnesium-assisted nitriding reaction using nitrogen gas (N 2 ) as the nitrogen source. Systematical studies were conducted to reveal the mechanism of magnesium-assisted nitriding process in constructing TiN nanostructures under N 2 atmosphere. The as-synthesized TiN NRs were directly used as the anodes for lithium ion batteries and delivered an excellent reversible capacity of 710 mAh g −1 at the current density of 100 mA g −1 after 200 cycles. In addition, the TiN NRs also exhibited excellent cycling stability and rate capability. Our work provides a low cost, environmental friendly and reliable strategy to synthesize TiN materials from TiO 2 by using N 2 as the nitrogen source, which may facilitate the practical applications of TiN materials in electrochemical/photo-electrochemical energy storage and conversion systems.
研究领域:
材料科学
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电化学能源存储
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DOI
高影响因子
ACS Omega
·
2022
·
IF 4.132
Zhisen He,Shanjian Liu,Wenjing Zhao,Mengqian Yin,Mei Jiang,Dongmei Bi
This study aimed to investigate the effect of the urea content on the characteristics and distribution of nitrogen-rich bio-oil and nitrogen-doped biochar. Cellulose, cellobiose, and glucose were used as feedstock. Urea was used as the exogenous nitrogen source in nitrogen-rich pyrolysis at 500 °C. The order of the nitrogen increase in the nitrogen-doped biochar was cellulose < cellobiose < glucose. Nitrogen-doped biochar consisted of abundant nitrogen and nitrogenous functional groups, and the stability of biochar was optimal. The nitrogen-doped biochar obtained from cellulose showed the optimal adsorption performance for diethyl phthalate with 50% urea addition. When the proportion of urea was 20%, the content of anhydro-sugars in bio-oil reached the maximum value (61.86%). Furans and other small-molecule oxygenates were intermediates to produce nitrogenous heterocyclic compounds (NHCs) from cellulose. When the proportion of urea was 40%, the bio-oil had the highest selectivity (91.63%) of NHCs. The NHCs in the obtained bio-oil mainly consisted of pyrroles, pyrimidines, pyridines, imidazoles, and pyrazines. Therefore, the excellent proportion of urea in the blend could promote the generation of high-value NHCs and nitrogen-doped biochar from the nitrogen-rich pyrolysis of cellulose (and its model compounds).
研究领域:
能源与环境科学
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生物质转化
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2018
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IF 3.235
Anran Liu,Mengyao Ma,Xiaoqin Zhang,Jing Ming,Ling Jiang,Ying Li,Yuanjian Zhang,Songqin Liu
Nitrogen doped carbon nanomaterials are excellent electrode materials and catalysts due to their extraordinary conductivity, prolific structures, and abundant active sites. Herein, two kinds of waste biomass, catkins and Okara were used as precursors for the preparation of novel nitrogen doped carbon fibers via hydrothermal and pyrolysis process . The blend of nitrogen-rich Okara with catkins effectively enhanced the content of doped nitrogen in the product. The as-prepared sample (denoted as NCF900) exhibited a hollow fiber like structure with a diameter of 2 to 5 μm and had abundant highly active sites of pyridinic N and graphitic N, thereby improving its electrocatalytic activity in oxygen reduction reaction (ORR). The typical rotating disk electrode test proved that the NCF900 exhibited a high onset potential (0.82 V vs RHE) and a nearly four-electron pathway for ORR in alkaline solution as well as stronger methanol tolerance and better long-term durability than commercial Pt/C. The green, low cost synthetic method and the excellent ORR catalytic efficiency of NCF900 made it a promising electrocatalytic material for the ORR in fuel cells.
研究领域:
材料科学
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能源科学
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环境科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
He Yingchun,Ma Dong-Dong,Ma Ke,Li Xiaofang,Han Lili,Wu Xin-Tao,Zhu Qi-Long
Electrochemically constructing C–N and N–C–N bonds provides an economical and sustainable alternative to conventional chemosynthesis. Herein, a hierarchically ordered open superstructure of N-doped carbon isolated with accessible three-coordinated Zn single-atom sites is explored for efficient electrocatalytic N–C–N coupling. Benefiting from the distinctive structural merits, this catalyst enables electrocatalytic preparation of N–C–N bonded compounds from methanol and amines. Notably, the Faradaic efficiency and selectivity of N,N,N’,N’ -tetramethyldiaminomethane reach up to 77% and 96% at 0.8 V, respectively. Further integrating the aminoalkylation reaction, an electro-thermo cascade synthesis is explored with the electrochemically obtained N,N,N’,N’ -tetramethyldiaminomethane serving as a unique reagent, leading to a specific set of organonitrogen compounds with (dimethylamino)methyl substituent, including topotecan hydrochloride, an anti-tumor drug, with a high yield of 95%. Furthermore, the in situ spectroscopic characterization and calculations unveil that the under-coordinated Zn-N 3 sites play a pivotal role in stabilizing the key *CH 2 O intermediate, thereby facilitating subsequent nucleophilic addition with amines.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 9
·5543-5553
·
IF 6.895
Shihong Wu,Ronghui Zhou,Hanjiao Chen,Jinyi Zhang,Peng Wu
Photosensitization is a promising avenue of oxygen activation, which can overcome the spin selection rule to transform the ground state oxygen (3O2) into a highly reactive singlet oxygen (1O2). Carbon dots (CDs) are a promising type of carbon-based photosensitizer, and nitrogen doping can further improve the oxygen photosensitization performance. Although the roles of nitrogen doping in tuning the optical properties (mainly absorption and fluorescence) of CDs have been well-studied, their association with oxygen photosensitization has not been reported. Herein, using the well-developed synthetic protocol of hydrothermal treatment of citric acid and ethylenediamine, we prepared nitrogen-doped CDs (N-CDs) of varied nitrogen contents. The oxygen photosensitization performances of the N-CDs were first confirmed by ROS investigation with TMB oxidation as the ROS probe and EPR. After XPS analysis of the surface nitrogen doping speciation, it was found that the changes of graphitic N and pyrrolic N correlated well with the oxygen photosensitization performances of N-CDs. Further theoretical calculations indicated that the two key factors for oxygen photosensitization, namely triplet activation and oxygen adsorption, are mainly associated with graphitic N and pyrrolic N, respectively. The results in this work help further understanding of the oxygen photosensitization mechanism of N-CDs, and are expected to be useful in the future design of carbon-based photosensitizers.
研究领域:
材料科学
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光化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Jia Shunhan,Zhang Libing,Liu Hanle,Wang Ruhan,Jin Xiangyuan,Wu Limin,Song Xinning,Tan Xingxing,Ma Xiaodong,Feng Jiaqi,Zhu Qinggong,Kang Xinchen,Qian Qingli,Sun Xiaofu,Han Buxing
Nitrogen oxides (NO x ) play important roles in the nitrogen cycle system and serve as renewable nitrogen sources for the synthesis of value-added chemicals driven by clean electricity. However, it is challenging to achieve selective conversion of NO x to multi-nitrogen products (e.g., N 2 H 4 ) via precise construction of a single N-N bond. Herein, we propose a strategy for NO x -to-N 2 H 4 under ambient conditions, involving electrochemical NO x upgrading to NH 3 , followed by ketone-mediated NH 3 to N 2 H 4 . It can achieve an impressive overall NO x -to-N 2 H 4 selectivity of 88.7%. We elucidate mechanistic insights into the ketone-mediated N-N coupling process. Diphenyl ketone (DPK) emerges as an optimal mediator, facilitating controlled N-N coupling, owing to its steric and conjugation effects. The acetonitrile solvent stabilizes and activates key imine intermediates through hydrogen bonding. Experimental results reveal that Ph 2 CN* intermediates formed on WO 3 catalysts acted as pivotal monomers to drive controlled N-N coupling with high selectivity, facilitated by lattice-oxygen-mediated dehydrogenation. Additionally, both WO 3 catalysts and DPK mediators exhibit favorable reusability, offering promise for green N 2 H 4 synthesis.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Fei Wang,Jianchun Jiang,Kui Wang,Qiaolong Zhai,Feng Long,Peng Liu,Junfeng Feng,Haihong Xia,Jun Ye,Jing Li,Junming Xu
The in situ polymerization of aniline as a nitrogen source was adopted to prepare nitrogen-doped mesoporous carbon (NMC), which further supported the molybdenum carbide catalyst for the hydrotreatment of fatty acids. The nitrogen doping drastically enhanced the catalytic performance of Mo 2 C/N 1.0 MC-700 with 92.7% conversion and 86.7% selectivity, which are much higher than the values of Mo 2 C/MC (84.8% and 70.1%, respectively). The kinetic study revealed that the apparent activation energy was reduced greatly after nitrogen doping. In addition, the nitrogen-doped catalyst showed decent stability, and the conversion and selectivity over Mo 2 C/N 1.0 MC-700 decreased by 4.4% and 6.9% respectively, after recycling three times. The deactivation mainly resulted from the coke deposition on the surface of catalyst. The high catalytic activity and stability were ascribed to the formation of pyridinic N and pyrrolic N in NMC, which resulted in the high dispersion of Mo, a decrease in the particle size as well as strong interactions between support and active sites. The hydrotreatment conditions of oleic acid were studied, and the optimal reaction conditions were as follows: reaction temperature, 350 °C; initial H 2 pressure, 3.0 MPa; n-hexane as solvent. Moreover, the results indicated that a substrate with a saturated carbon double bond and ester group was more easily converted into hydrocarbons.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
Advanced Materials Interfaces
·
2018
·Vol. 5
·期 23
·1801149
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IF 4.834
Shuguang Wang,Jinwen Qin,Lirong Zheng,Donglei Guo,Minhua Cao
Controllable synthesis of 2D carbon nanosheets with high heteroatom-doping level, large specific surface area, and hierarchically pore structure is difficult and desired. In this work, a novel and simple self-sacrificing in situ formed dual-template strategy is first developed to synthesize N/S codoped hierarchically porous carbon nanosheets. The in-situ formed g -C 3 N 4 and amorphous ZnO act as self-sacrificing templates on account of their thermal decomposition and evaporation at higher temperature. The N/S codoped hierarchically porous carbon nanosheets simultaneously possess high heteroatom-doping level (N: 10.51 wt%; S: 1.71 wt%), large specific surface area (904.63 m 2 g −1 ), and abundant hierarchically porous structure. Particularly, this material possesses a high content of pyridinic-N and pyrrolic-N configuration (65.66%). These unique structure advantages of N/S codoped hierarchically porous carbon nanosheets contribute to high oxygen reduction electrocatalytic activity in both basic and acidic environments. Additionally, as the anode material for sodium-ion batteries, the material also displays a high reversible capacity of 270.1 mAh g −1 at a current density of 100 mA g −1 and high stability (160.1 mAh g −1 after 2000 cycles at 1000 mA g −1 with a capacity retention of 82.3%). These results indicate a great potential of the material in energy conversion and storage applications.
研究领域:
材料科学
·
能源化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）