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ENERGY & FUELS · 2023 · IF 5.3

Effect of Heteroatoms on Pseudocapacitance for N/O Co-doped Porous Carbon in an Alkaline Aqueous Electrolyte

Weiwei Zhu,Dekui Shen,Haijiao Xie

The primary objective of this investigation is to assess the electrochemical properties of porous carbon, concurrently doped with nitrogen and oxygen, featuring a diverse array of surface heteroatoms. We synthesized this type of porous carbon material from Houttuynia cordata, subjected to procedures of nitrogen infusion and activation. Our findings indicate a strong relationship between the pseudocapacitance of the dually doped porous carbon and the concentration of pyridinic-nitrogen. As the pyridinic-nitrogen content increases, the pseudocapacitance first increases due to the growing tendency of active sites. After the pyridinic-nitrogen/carbon atomic ratio reaches 0.027, the pseudocapacitance decreases because the conductivity of the carbon material decreases. Density functional theory simulations indicate that the band gap of pyridinic-nitrogen-doped graphene is 0.021 eV, which is larger than that of nitrogen-free graphene. The increased band gap makes electronic transitions less likely, and the conductivity decreases.

研究领域: 材料科学 · 电化学
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CARBON · 2021 · IF 9.594

Gelatin-derived carbon: Carbonization mechanism and application in K-ion storage

Na Yang,Rong Shao,Zhengping Zhang,Meiling Dou,Jin Niu,Feng Wang

Gelatin, a natural macromolecular substance formed by the hydrolysis of collagen, offers the advantages of abundant resources and low cost. It is a good precursor for the synthesis of N, O-doped carbon materials. Although some gelatin-derived carbon materials have been used for electrochemical energy storage , there have been few studies for the mechanism of gelatin carbonization . In addition, the influence of heteroatoms and defects on the K-ion storage performance remains unclear. In this work, in situ and ex situ characterization methods have been used to study the mechanism of gelatin carbonization. The pathways leading to formation of the carbon framework, heteroatom doping and defect generation in gelatin-based carbons during the pyrolysis process have been clearly identified. Moreover, by means of DFT calculations and experimental measurements, it has been confirmed that heteroatoms and defects both play important roles in improving the storage performance of potassium ions. By virtue of its abundance of both heteroatoms and defects, our optimized anode shows better electrochemical performance than graphite anodes. This study not only clarifies our understanding of carbonization mechanism and mechanism of K-ion storage in carbon materials, but also provides pathways for the synthesis and applications of new carbon-based anode materials for alkali-ion batteries.

CAS / MDL: 9000-70-8
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

New insight into the heteroatom-doped carbon as the electrode material for supercapacitors

Yutong Li,Su Zhang,Huaihe Song,Xiaohong Chen,Jisheng Zhou,Song Hong

Heteroatom-doped carbon with 4.06% of nitrogen and 10.42% of oxygen was synthesized by pyrolysis of ortho-aminophenol/formaldehyde resin. After high temperature hydrogen reduction, 2.22% of the surface oxygen was removed while the nitrogen content remained almost no change. The specific surface area enlarged from 90   m 2   g −1 to 226   m 2   g −1 and abundant micropores appeared. But we found that the specific capacitance of the reduced carbon as electrode for supercapacitors was decreased nearly 25 %. By measuring the conductivity, surface wettability, and electrochemical impedance, we proposed that (a) surface oxygen played an important role in the capacitive performance, especially the pseudocapacitance; (b) though the doped-oxygen reduced the electronic conductivity, on the other hand, enhanced the surface wettability and ion diffusion rate of the carbon electrodes.

CAS / MDL: 95-55-6
研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Precise control of platinum coordination environment on fullerene-derived catalysts for oxygen reduction reaction

Hua Pan,Xinxing Zhan,Chao Wang,Juan Tian,Zijian Gao,Lingyun Zhou,Yadian Xie,Xin Tong

The interaction between catalysts and supports is recognized as a crucial factor influencing catalytic activity and stability. However, the carbon materials, which have been widely employed as the support at present, encounter challenges including intricate composition and the difficulty of precise control. In this study, the fullerene-derived carbon materials serve as support to electrocatalysts with low platinum. Fullerene-based materials, as the only carbon material with a well-defined molecular structure, have a controllable active site structure, which can provide a reaction model for studying metal-support interactions. Four kinds of fullerene-derived catalysts such as Pt/fullerene, Pt/nitrogen-doped fullerene, Pt/sulfur-doped fullerene, and Pt/phosphorus-doped fullerene, were synthesized. Once the coordination environment of the Pt particles was controlled, thus their catalytic performance was modulated. Despite a platinum loading of only 4.2%, Pt/N-fullerene demonstrates superior oxygen reduction activity and stability compared to commercial Pt/C (20%). Density functional theory calculations show that the introduction of heteroatoms can change the surface charge distribution of fullerenes, in which N-fullerene has a more negative electrostatic potential and can effectively anchor Pt. This research establishes a foundation for understanding the catalysts-support interaction and further precise control of the coordination environment of Pt. This provides new insights for designing efficient ORR catalysts.

CAS / MDL: 83-86-3
研究领域: 材料科学 · 电化学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2025 · IF 4.6

Ultra-stable room temperature phosphorescence CDs-based composite materials for anti-counterfeiting application

Wenli Feng,Lu Zhao,Chenxia Hao,Lin Yuan,Lizhen Liu,Xiaoming Yang,Yunfeng Bai,Feng Feng

Counterfeit and shoddy products exist widely in our daily life. Effective anti-counterfeiting means have become an issue with increasing concern. Herein, we proposed a new strategy for dispersing N, S-CDs into melamine phosphate (MP) to prepare N, S-CDs@MP composite. The co-doping of carbon dots with heteroatoms (N and S atoms) in conjunction with matrix protection synergistically enhanced the emission of long-lived room temperature phosphorescence (RTP). The obtained N, S-CDs@MP composite exhibited green RTP with phosphorescence quantum yield of 9.27 % and lifetime of 489 ms. More importantly, even in extreme conditions, the RTP of N, S-CDs@MP in the dispersion still persisted. The excellent RTP properties and good stability made N, S-CDs@MP a promising material for advanced anti-counterfeiting applications. This study afforded a new RTP material which could be easily prepared and used for information encryption and graphic anti-counterfeiting.

CAS / MDL: 20208-95-1
研究领域: 材料科学 · 光学
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Catalysts · 2021 ·Vol. 11 ·期 2 ·169 · IF 4.146

A “Superaerophobic” Se-Doped CoS2 Porous Nanowires Array for Cost-Saving Hydrogen Evolution

Yan Tan,Yijun Yin,Xianhong Yin,Chenghao Lan,Yu Wang,Feilong Hu,Qin Huang,Yan Mi

The pursuit of low-cost and high-efficiency catalyst is imperative for the development and utilization of hydrogen energy. Heteroatomic doping which is conducive to the redistribution of electric density is one of the promising strategies to improve catalytic activity. Herein, the Se-doped CoS2porous nanowires array with a superaerophobic surface was constructed on carbon fiber. Due to the electronic modulation and the unique superaerophobic structure, it showed improved hydrogen evolution activity and stability in urea-containing electrolyte. At a current density of 10 mA cm−2, the overpotentials are 188 mV for hydrogen evolution reaction (HER) and 1.46 V for urea oxidation reaction (UOR). When it was set as a cell, the voltage is low as 1.44 V. Meanwhile, the current densities of HER and UOR, as well as of cell remained basically unchanged after a continuous operation for 48 h. This work opens up a new idea for designing of cost-saving hydrogen evolution electrocatalysts.Keywords:superaerophobic;cost-saving hydrogen evolution;heteroatom doping;electronic adjustment

研究领域: 材料科学 · 能源化学
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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Substantial Role of Nitrogen and Sulfur in Quaternary-Atom-Doped Multishelled Carbon Nanospheres for the Oxygen Evolution Reaction

Yasir Abbas,Majid Basharat,Wei Liu,Muhammad Shuaib Khan,Shuangkun Zhang,Shafqat Ali,Zhanpeng Wu,Dezhen Wu

The synergy between nitrogen (N) and sulfur (S) in quaternary heteroatom-doped carbons is rarely probed, although these elements can significantly alter the performance of the oxygen evolution reaction (OER). Herein, quaternary heteroatom (N, S, P, O)-doped multishelled carbon (NSPO-C) nanospheres are synthesized from heteroatom-containing poly(cyclotriphosphazene-codioxo-thiane) (PCD) polymer nanospheres. The contents of these quaternary heteroatoms were controlled via a facile carbonization process. The OER performance was tested, which was found to be related to the N and S contents, and the as-prepared NSPO-C-8 nanosphere anode with optimized contents of N (2.76 wt %) and S (1.52 wt %) showed a maximum OER activity, that is, it required a very low overpotential of 339 mV to obtain a current density of 10 mA cm–2 with a low Tafel slope value (39.40 mV dec–1), which is much lower than its conventional RuO2 (401 mV), 20% Pt/C (566 mV), and PO-C nanosphere (452 mV) counterparts. Higher performance is attributed to the synergy between N and S in the NSPO-C nanospheres, which provides maximum exposure to electroactive sites, while special morphology ensures efficient pathways for fast charge transportation. These findings advocate that polyphosphazene-derived heteroatom-doped carbons are potential candidates to fabricate high-performance devices for water oxidation.

CAS / MDL: 942947-94-6
研究领域: 材料科学 · 电化学
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Catalysts · 2023 ·Vol. 13 ·期 3 ·532 · IF 3.9

Effect of Pyrolysis Conditions on the MOFs-Derived Zinc-Based Catalysts in Acetylene Acetoxylation

Guowang Shen,Mengli Li,Yuhao Chen,Zhuang Xu,Xugen Wang,Bin Dai

The preparation method and calcination temperature of metal-organic framework (MOFs)-derived materials are critical factors affecting catalytic performance. In this work, the preparation conditions of MOFS precursors were optimized, and zinc-based catalysts with different activities (MOF5-700, MOF5-750, and MOF5-800) were obtained by pyrolysis of MOFS precursors under nitrogen, which were then applied to an acetylene acetoxylation reaction system. According to the results, the conversion rate of acetic acid under catalysis was significantly different. (MOF5-700 (48%), MOF5-750 (62%), and MOF5-800 (22%)). Comparing the activity of the catalyst with the industrial catalyst Zn(OAc)2/AC (20%), MOF5-750 showed higher activity, and the acetic acid conversion rate remained around 60% after 50 h of stability testing. By characterization analysis, MOFs-derived materials were obtained after proper temperature pyrolysis. They have high mesoporous content, defects, and oxygen-containing functional groups and can maintain a good crystal structure, greatly reducing the loss of active components. This is the main reason for the good performance of the MOF5-750 catalyst in acetylene acetoxylation. Thus, the preparation conditions and favorable pyrolysis temperature of MOF derivative catalysts play a key role in the catalytic performance of acetylene acetoxylation.Keywords:metal–organic frameworks;heteroatoms;acetylene acetoxylation;pyrolysis

CAS / MDL: 100-21-0
研究领域: 催化 · 化学工程 · 材料科学
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WOOD SCIENCE AND TECHNOLOGY · 2023 ·Vol. 57 ·期 4 ·879-901 · IF 3.4

Facile one-step synthesis of cork-derived hierarchical porous carbons with P, N, and O heteroatoms for high-performance supercapacitor electrodes

Luo Lingcong,Zhang Qianqian,Lan Yuling,Deng Jianping,Lin Yang,Du Guanben,Zhao Weigang

High-performance electrodes of activated carbons (PNOACs) with P, N, and O heteroatoms were prepared through a simple one-step phosphoric acid activation method without the need for any dopants or post-treatment. In the preparation procedure, cork biomass material from Quercus variabilis was used as the precursor, and phosphoric acid was used as both the phosphoric resource and the activation agent. The pore structure, morphology, and physicochemical properties of the as-prepared carbons were investigated. In addition, the electrochemical performances of the PNOACs were evaluated using three-electrode and two-electrode systems (symmetric supercapacitor, AS). The results indicated that cork is promising as a low-cost and environmental-friendly precursor for producing high-performance supercapacitors electrode. Furthermore, galvanostatic charge–discharge analysis revealed a specific capacitance of 206 F g −1 at a current density of 0.5 A g −1 , which can be attributed to the excellent hierarchical pore structure (micro-, meso-, and macropores) and suitable pore size distribution of the PNOACs. The specific surface area and total pore volume as high as 515.80 m 2  g −1 and 0.29 cm 3  g −1 were obtained, respectively. The presence of heteroatoms, namely N (0.81–1.07%), P (0.52–2.06%), and O (15.87–19.18%) content, on the carbon surface resulted in a considerable enhancement in the capacitive performance. Furthermore, a PNOAC sample, prepared at 600 °C with a mass ratio of 1:1, exhibited high long-term cycling stability (84.5%) and an energy density of 15.03 W h kg −1 . Therefore, cork is highly promising as an electrode material for supercapacitors to attain exceptional electrochemical performance, as well as provide a new possibility for the utilization and valorization of high-value cork waste.

CAS / MDL: 7664-38-2
研究领域: 材料科学 · 能源存储 · 环境科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2023 · IF 3.3

Sulfonated heteroatom co-doped carbon materials with a porous structure boosting electrosorption capacity for uranium (VI) removal

Ruiming Zhang,Luowen Xu,Fengtao Yu,Saijin Xiao,Changfu Wang,Dingzhong Yuan,Yan Liu

The discharge of effluents containing radionuclides has a detrimental impact on the ecological environment, emphasizing the importance of recovering U(VI) from nuclear wastewater to safeguard the environment. Electrosorption has emerged as a viable technique for the extraction of uranium from radioactive solutions. Herein, we propose a facile strategy utilizing ultrasonication to fabricate a novel sulfonated carbon material (HCCMs-SO 3 H) co-doped with B, N, and P atoms. The incorporation of sulfonate groups and doping heteratoms in HCCMs-SO 3 H significantly enhanced its electrosorption capacity for uranium, yielding an impressive capacity of 626.37 mg/g at 0.9 V. This enhancement in electrosorption ability is attributed to the synergistic effects of sulfonate groups and the presence of B, N, and P atoms in the carbon matrix. Furthermore, HCCMs-SO 3 H exhibited excellent recoverability and selectivity towards uranium, endowing it a promising material for uranium extraction from uranium-containing solutions. Its high electrosorption capacity, coupled with favorable recoverability and selectivity, positioned HCCMs-SO 3 H as a potential candidate for efficient and environmentally friendly uranium recovery processes.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ORGANIC CHEMISTRY · 2019 · IF 4.745

Organocatalytic Asymmetric α-Sulfenylation of 2-Substituted Indolin-3-ones: A Strategy for the Synthesis of Chiral 2,2-Disubstituted Indole-3-ones with S- and N-Containing Heteroquaternary Carbon Stereocenter

Yong-Long Zhao,Xing-Hai Fei,Yong-Qin Tang,Peng-Fei Xu,Fen-Fen Yang,Bin He,Xiao-Zhong Fu,Yuan-Yong Yang,Meng Zhou,Yuan-Hu Mao,Yong-Xi Dong,Chun Li

An organocatalytic asymmetric α-sulfenylation of 2-substituted indolin-3-ones with N-(alkylthio or arylthio)succinimides has been developed for the first time using Cinchona-derived squaramide as the catalyst. Various chiral 2,2-disubstituted indole-3-ones with S- and N-containing heteroquaternary carbon stereocenters were obtained with up to 98% yield and 99% ee.

研究领域: 有机化学 · 合成化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Synthesis of heteroatom zeolite subcrystals as catalytic materials and structural building blocks

Ke Du,Jiayu Yu,Pingping Wang,Di Pan,Zhaoqi Ye,Wanyi Li,Ling Ding,Wei Chen,Yi Tang,Yahong Zhang

Recent advancements in zeolite synthesis techniques have facilitated the synthesis of heteroatom zeolites with customized acidity and redox properties. However, challenges remain in controlling the content, accessibility and distribution of active center. A new zeolite construction strategy is still desired for the design of effective heteroatom zeolite catalysts. In this work, we synthesized and extracted a series of highly short-range ordered heteroatom-containing MFI zeolite subcrystals (Al, Ga, Ti, Zn, and Sn) with open framework structures and tunable acidic properties. These heteroatom-containing zeolite subcrystals not only acted as catalyst materials with diverse catalytic activity and high active site accessibility, but also served as versatile building blocks for customized zeolite synthesis and active site modulation via non-classical aggregation and cross-aggregation crystallization processes. Notably, we demonstrated that the catalytic performance of the unique subcrystals and their aggregated products were tailored to meet the specific requirements of reactions such as olefin epoxidation and macromolecular cracking. Furthermore, this synthesis strategy was also applicable to the synthesis of MEL zeolite subcrystals. The continuous expansion of subcrystal category opens new avenues for the design of multifunctional zeolite catalysts, contributing valuable insights into zeolite synthesis and active site regulation.

CAS / MDL: 10026-06-9 717-74-8
研究领域: 材料科学 · 催化化学
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