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Self-sacrificial template synthesis of Fe, N co-doped porous carbon as efficient oxygen reduction electrocatalysts towards Zn-air battery application 被引量:1
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作者 Tianfang Yang Ye Chen +2 位作者 Yang Liu Xupo Liu Shuyan Gao 《Chinese Chemical Letters》 SCIE CAS CSCD 2022年第4期2171-2177,共7页
Designing highly efficient non-precious based electrocatalysts for oxygen reduction reaction(ORR) is of significance for the rapid development of metal-air batteries.Herein,a hydrothermal-pyrolysis method is employed ... Designing highly efficient non-precious based electrocatalysts for oxygen reduction reaction(ORR) is of significance for the rapid development of metal-air batteries.Herein,a hydrothermal-pyrolysis method is employed to fabricate Fe,N co-doped porous carbon materials as effective ORR electrocatalyst through adopting graphitic carbon nitride(g-C_(3)N_(4)) as both the self-sacrificial templates and N sources.The gC_(3)N_(4)provides a high concentration of unsaturated pyridine-type N to coordinate with iron to form Fe-N active sites.Through adjusting the Fe doping amounts,it is proved that appropriate Fe doping content is conducive to the construction of abundant defects and active sites of Fe-N.The as-prepared catalyst exhibits superior electrocatalytic ORR performance in alkaline media with half-wave potential(E_(1/2)=0.82 V) and onset potential(E_(onset)=0.95 V),equivalent to the commercial Pt/C catalyst.Moreover,there is almost no activity loss after 10 k continuous cyclic voltammetry cycles and methanol tolerance,indicating the excellent durability and superior methanol tolerance.Remarkably,when assembled as the cathode in a Zn-air battery,the device displays a power density of 99 mW/cm^(2),an open-circuit potential of 1.48 V and long-term discharge-charge cycling stability,indicating the promising potential to substitute the Pt catalyst for practical application. 展开更多
关键词 ELECTROCATALYsT Oxygen reduction reaction fe n co-doped porous carbon fe-n active sites Zn-air batteries
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Fe/Fe2O3 nanoparticles anchored on Fe-N-doped carbon nanosheets as bifunctional oxygen electrocatalysts for rechargeable zinc-air batteries 被引量:12
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作者 Yipeng Zang Haimin Zhang +5 位作者 Xian Zhang Rongrong Liu Shengwen Liu Guozhong Wang Yunxia Zhang Huijun Zhao 《Nano Research》 SCIE EI CAS CSCD 2016年第7期2123-2137,共15页
Electrocatalysts with high catalytic activity and stability play a key role in promising renewable energy technologies, such as fuel cells and metal-air batteries. Here, we report the synthesis of Fe/Fe203 nanoparticl... Electrocatalysts with high catalytic activity and stability play a key role in promising renewable energy technologies, such as fuel cells and metal-air batteries. Here, we report the synthesis of Fe/Fe203 nanoparticles anchored on Fe-N-doped carbon nanosheets (Fe/Fe2Og@Fe-N-C) using shrimp shell-derived N-doped carbon nanodots as carbon and nitrogen sources in the presence of FeCI3 by a simple pyrolysis approach. Fe/Fe203@Fe-N-C obtained at a pyrolysis temperature of 1,000 ℃ (Fe/Fe2OB@Fe-N-C-1000) possessed a mesoporous structure and high surface area of 747.3 m2-g-1. As an electrocatalyst, Fe/Fe203@Fe-N-C-1000 exhibited bifunctional electrocatalytic activities toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline media, com- parable to that of commercial Pt/C for ORR and RuO2 for OER, respectively. The Zn-air battery test demonstrated that Fe/Fe2OB@Fe-N-C-1000 had a superior rechargeable performance and cycling stability as an air cathode material with an open drcuit voltage of 1.47 V (vs. Ag/AgCl) and a power density of 193 mW.cm-2 at a current density of 220 mA-cm-2. These performances were better than other commercial catalysts with an open circuit voltage of 1.36 V and a power density of 173 mW-cm^-2 at a current density of 220 mA.cm-2 (a mixture of commercial Pt/C and RuO2 with a mass ratio of 1:1 was used for the rechargeable Zn-air battery measurements). This work will be helpful to design and develop low-cost and abundant bifunctional oxygen electrocatalysts for future metal-air batteries. 展开更多
关键词 n-doped carbon nanodots fe/fe2O3@fe-n-dopedcarbon oxygen reduction reaction oxygen evolution reaction rechargeable zinc-airbattery
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Development of nitrogen and sulfur-doped carbon dots for cellular imaging 被引量:6
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作者 Hui Liu Yue Zhang Chengzhi Huang 《Journal of Pharmaceutical Analysis》 SCIE CAS CSCD 2019年第2期127-132,共6页
Heteroatom-doped carbon dots(CDs) have attracted extensive interest because of their improved electronic and fluorescence properties with heteroatom doping. In this study, a new synthetic method for nitrogen(N) and su... Heteroatom-doped carbon dots(CDs) have attracted extensive interest because of their improved electronic and fluorescence properties with heteroatom doping. In this study, a new synthetic method for nitrogen(N) and sulfur(S)-doped CDs was developed via a hydrothermal method using methionine and citric acid as raw materials. The as-prepared CDs exhibit excellent optical properties and good biocompatibility. The spherical N,S-doped CDs have an average diameter of 5 nm. They consist of C, O, N and S, and take on excellent water solubility due to the hydroxyl and carboxyl, amino groups on the surface.The CDs have a photoluminescence quantum yield of 13.8% using quinine sulfate as a reference; the average fluorescence lifetime of the CDs was 3.67 ns. The CDs solution present good photoluminescence properties, and the maximum excitation wavelength and emission wavelength locate at 330 nm and405 nm, respectively. In addition, their fluorescence intensity almost does not change under the conditions of acid, alkali, and high salt, which indicated their anti-photobleaching property and good light stability. Based on the good biocompatibility and strong fluorescence emission of the CDs, they can be used as fluorescent imaging reagents. 展开更多
关键词 n s-doped carbon DOTs FLUOREsCEnT REAGEnT Cellular imaging
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Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery 被引量:4
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作者 Hao Fan Yu Wang +8 位作者 Fujie Gao Longqi Yang Meng Liu Xiao Du Peng Wang Lijun Yang Qiang Wu Xizhang Wang Zheng Hu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第7期64-71,共8页
Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hier... Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries. 展开更多
关键词 3D HIERARCHICAL carbon nAnOCAGEs s n CO-DOPInG BIFUnCTIOnAL electrocatalysis Zn-air battery
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S掺杂促进Fe/N/C催化剂氧还原活性的实验与理论研究 被引量:3
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作者 陈驰 张雪 +2 位作者 周志有 张新胜 孙世刚 《物理化学学报》 SCIE CAS CSCD 北大核心 2017年第9期1875-1883,共9页
向Fe/N/C非贵金属催化剂中再引入S掺杂是进一步提高其氧还原催化活性的有效方法。为了探究活性提高的原因,本文以三聚氰胺-甲醛树脂为前驱体,氯化钙为模板,氯化铁为铁源,通过添加硫氰化钾(KSCN)来控制热解催化剂的S掺杂量。通过对比分... 向Fe/N/C非贵金属催化剂中再引入S掺杂是进一步提高其氧还原催化活性的有效方法。为了探究活性提高的原因,本文以三聚氰胺-甲醛树脂为前驱体,氯化钙为模板,氯化铁为铁源,通过添加硫氰化钾(KSCN)来控制热解催化剂的S掺杂量。通过对比分析催化剂的物化性质,结合密度泛函理论(DFT)计算,分析S掺杂促进Fe/N/C催化剂氧还原活性的原因。透射电子显微镜(TEM)和N_2吸脱附等温线测试结果表明,S元素可抑制含铁纳米粒子的形成,促使形成多孔碳结构,提高比表面积。X射线光电子能谱(XPS)结果表明,适量S前驱体可实现较高的S掺杂含量,得到最优的活性,过量的S反而会导致Fe和S的掺杂量同时降低,影响活性。DFT计算结果表明在Fe-N_4大环中引入S掺杂,可增强O_2分子和中间体OOH与Fe-N_4结构中的Fe的相互作用,促进形成Fe―O键,从而导致O―O键的键能显著降低,为后续反应O―O键的断裂提供可能,促进ORR反应的进行。 展开更多
关键词 氧还原反应 非贵金属催化剂 fe/n/C材料 s掺杂 密度泛函理论
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Fe^(3+)及S-N共掺杂TiO_2纳米材料的制备及其光催化性能 被引量:2
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作者 苏碧桃 邓超 +3 位作者 费鹏 张春娥 陈亚丽 钟明 《西北师范大学学报(自然科学版)》 CAS 北大核心 2012年第5期48-52,71,共6页
以硫脲、硝酸铁、钛酸四丁酯分别作S、N、Fe和Ti源,利用sol-gel法制备了一系列Fe3+和S-N掺杂的TiO2光催化纳米材料(Fe3+/TiO2、S-N/TiO2、Fe3+/S-N/TiO2).利用X射线光电子能谱(XPS)、X射线衍射(XRD)、透射电镜(TEM)、紫外-可见光谱(UV-V... 以硫脲、硝酸铁、钛酸四丁酯分别作S、N、Fe和Ti源,利用sol-gel法制备了一系列Fe3+和S-N掺杂的TiO2光催化纳米材料(Fe3+/TiO2、S-N/TiO2、Fe3+/S-N/TiO2).利用X射线光电子能谱(XPS)、X射线衍射(XRD)、透射电镜(TEM)、紫外-可见光谱(UV-Vis)等技术进行表征,以亚甲基蓝(MB)的降解为模型反应,评价样品的光催化性能.结果表明,Fe3+、S-N的共掺杂将TiO2的光谱响应范围拓宽到可见区,使TiO2在紫外和太阳光下的催化活性得到显著改善,MB溶液在各样品上的催化降解脱色速率常数k1分别为:0.17(TiO2)、0.22(S-N/TiO2)、0.32(Fe3+/TiO2)和0.42h-1(Fe3+/S-N/TiO2),共掺杂材料Fe3+/S-N/TiO2的高催化活性归因于掺入的Fe3+和S-N协同作用的结果. 展开更多
关键词 TIO2 fe3%PLUs%-s-n共掺杂 sOL-GEL法 光催化性能 协同作用
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Implanting Ni into N-doped puffed carbon: A new advanced electrocatalyst for oxygen evolution reaction 被引量:1
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作者 Feng Cao Guoxiang Pan +1 位作者 Yujian Zhang Xinhui Xia 《Chinese Chemical Letters》 SCIE CAS CSCD 2020年第9期2230-2234,共5页
Tailored design and synthesis of high-quality electrocatalysts is vital for the advancement of oxygen evolution reaction(OER).Herein,we report a powerful puffing method to fabricate hierarchical porous N-doped carbon ... Tailored design and synthesis of high-quality electrocatalysts is vital for the advancement of oxygen evolution reaction(OER).Herein,we report a powerful puffing method to fabricate hierarchical porous N-doped carbon with numerous embedded Ni nanoparticles.Interestingly,during the puffing and annealing process,rice precursor with N and Ni sources can be in-situ converted into Ni-embedded N-doped porous carbon(N-PC/Ni) composite.The obtained N-PC/Ni composite possesses a cross-linked porous architecture containing conductive carbon backbone and active Ni nanoparticles electrocatalysts for OER.The pore formation in N-PC/Ni composite is also proposed because of carbothermic reduction.The N-PC/Ni composite is fully studied as electrocatalysts for OER.Due to increased active surface area,enhanced electronic conductivity and reactivity,the designed N-PC/Ni composite exhibits superior OER performance with a low Tafel slope(~88 mV/dec) and a low overpotential as well as excellent long-term stability in alkaline solution.Our proposed rational design strategy may provide a new way to construct other advanced metal/heteroatom-doped composites for widespread application in electrocatalysis. 展开更多
关键词 Oxygen evolution reaction ELECTROCATALYsIs porous carbon Metal-carbon composites n doping
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氮掺杂多孔碳负载Fe纳米颗粒用于高性能电催化还原CO_(2)与Zn-CO_(2)电池 被引量:2
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作者 杨文倩 薛自前 +9 位作者 杨俊 冼家慧 刘庆林 范雅楠 郑凯 廖锫钦 苏徽 刘庆华 李光琴 苏成勇 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2023年第5期185-194,共10页
电催化CO_(2)还原为CO因其技术与经济上的可行性而被认为是推进碳中和最有前景的反应之一.然而,水溶液中激烈的竞争性析氢反应阻碍生成单一高选择性产物.目前,贵金属纳米催化剂表现出较好的CO选择性,但稀缺性和高成本限制了其进一步应用... 电催化CO_(2)还原为CO因其技术与经济上的可行性而被认为是推进碳中和最有前景的反应之一.然而,水溶液中激烈的竞争性析氢反应阻碍生成单一高选择性产物.目前,贵金属纳米催化剂表现出较好的CO选择性,但稀缺性和高成本限制了其进一步应用.Fe纳米颗粒(NPs)具有电催化活性,且储量丰富成本低,被认为是一种潜在可替代贵金属的电催化剂,但Fe存在易氧化、团聚、稳定性差、吸附CO_(2)能力低等问题.因此,探索同时具有良好活性和稳定性的新型Fe NPs催化剂仍具有重要意义.金属-有机骨架(MOFs)衍生物被认为是合成锚定和激活金属纳米颗粒的良好前驱体.因此,将Fe NPs固定在MOFs衍生物中为开发稳定、高活性的Fe NPs催化剂提供了可行的机会.本文通过修饰MOFs前驱体的策略,对IRMOF-3(Zn)进行少量含铁配体单羧酸二茂铁的取代,结合一步热解碳化,制备了Fe NPs负载在海绵状氮掺杂多孔碳的复合催化剂(Fe@NPC).同时对配体为对苯二甲酸的MOF-5和配体为2-氨基-对苯二甲酸的IRMOF-3(Zn)进行热解碳化,制备了对照样品多孔碳MOF-5-D和氮掺杂多孔碳IRMOF-3-D.光电子能谱(XPS)和X射线吸收精细结构谱(XAFS)结果表明,在Fe@NPC中含有大量的Fe-Fe键以及极少量的Fe-N/C键,说明Fe主要以纳米颗粒形式存在,少量Fe-N/C分布在Fe NPs表面,在Fe NPs与氮掺杂碳基底间起到良好的连接作用.此外,Fe@NPC具有较大的比表面积(1264 m^(2)g^(-1))和高于MOF-5-D与IRMOF-3-D的CO_(2)吸附能力(93.5 cm^(3)g^(-1)),这种具有CO_(2)强吸附和丰富活性位点的多级孔结构为加速传质、加快CO_(2)转化奠定了良好的基础.在H-cell与-0.6 V_(RHE)的条件下,IRMOF-3-D的最大CO法拉第效率(FECO)为65.3%,是MOF-5-D(49.9%)的1.3倍,说明氮掺杂在一定程度上促进了CO_(2)的电还原.此外,Fe@NPC在-0.3 V_(RHE)到1.0 V_(RHE)的宽电位化学区间均表现出较好的性能,即最大的电流密度,最低的起始电位以及92.1%的最高的FECO.而且Fe@NPC在流动池中可以获得更高的FECO(96.4%),同时能够在H-cell与流动池中均保持良好的稳定性.由于*COOH高能垒,它的产生被认为是高效电化学CO_(2)-CO转换的瓶颈.进一步采用原位衰减全反射-傅里叶变换红外(ATR-IR)来实时监测中间体,并深入探究Fe@NPC作用于CO_(2)还原过程的机理,观测到中间体*COOH的逐渐形成和积累,以及同一反应时间内*COOH在Fe@NPC上的更快动力学形成过程;进一步说明Fe位点与氮掺杂多孔碳之间的协同作用显著提高了Fe@NPC的CO_(2)的捕获能力和传质能力并加速了CO生成的动力学.本文以Fe@NPC为阴极组装了Zn-CO_(2)电池,发现该电池具有良好的充电放电性能,放电过程中可提供3.0 mW cm^(-2)的峰值功率密度,同时表现出良好的稳定性(120个循环),实现CO_(2)电还原与储能的良好结合,并表现出高效的能量转换装置的良好应用潜力.综上,本文为设计用于高选择性的CO_(2)还原反应和能量转换器件的铁基催化剂提供了一种新方法. 展开更多
关键词 fe纳米颗粒 MOFs衍生物 氮掺杂多孔碳 CO_(2)电催化 Zn-CO_(2)电池
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三聚氰胺衍生的高石墨氮中空管状Fe-N/C催化碱性氧还原反应
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作者 赵晓琦 李晶 +3 位作者 张雪 李盈霄 高艳芳 刘玲 《内蒙古工业大学学报(自然科学版)》 2023年第4期309-317,共9页
以煅烧三聚氰胺后形成的C3N4材料为氮源,柠檬酸为碳源,六水合三氯化铁为铁源,通过两步法合成FeN/C催化剂,并考察该催化剂对氧还原反应的电催化能力。采用XRD、SEM、Raman、XPS等表征手段对Fe-N/C催化剂的晶体结构和元素化学状态进行综... 以煅烧三聚氰胺后形成的C3N4材料为氮源,柠檬酸为碳源,六水合三氯化铁为铁源,通过两步法合成FeN/C催化剂,并考察该催化剂对氧还原反应的电催化能力。采用XRD、SEM、Raman、XPS等表征手段对Fe-N/C催化剂的晶体结构和元素化学状态进行综合评价;以CV和LSV等电化学测试手段探究Fe-N/C催化剂的氧还原电催化能力。研究结果表明,Fe-N/C催化剂具有管状形貌、较高的石墨氮含量和较佳的氧还原电催化能力。通过对电化学性能关键参数进行分析发现,Fe-N/C催化剂的起始电位是1.071 V vs. RHE,半波电位是0.911 V vs. RHE,极限电流密度是5.943 mA/cm2。 展开更多
关键词 氧还原反应 燃料电池 fe-n/C催化剂 空心管电催化剂 氮掺杂碳
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微波绿色合成N,S共掺杂碳点及其在Fe^(3+)检测和温度传感方面的应用 被引量:5
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作者 陈文静 伍贤学 +6 位作者 吴云英 李亮星 肖群 雷旭 罗义 鄢林琼 谢建新 《中国测试》 CAS 北大核心 2021年第3期64-69,共6页
以韭菜为前驱体,采用微波法一步绿色合成N,S共掺杂的粒径均匀、分散性好的碳点。所合成的碳点近似球状,粒径2.0-5.0 nm。在365 nm的紫外灯照射下发明亮的蓝色荧光,发射峰具有激发波长依赖性。Fe^(3+)对所制备的碳点有明显选择性荧光猝... 以韭菜为前驱体,采用微波法一步绿色合成N,S共掺杂的粒径均匀、分散性好的碳点。所合成的碳点近似球状,粒径2.0-5.0 nm。在365 nm的紫外灯照射下发明亮的蓝色荧光,发射峰具有激发波长依赖性。Fe^(3+)对所制备的碳点有明显选择性荧光猝灭现象。在5-300μmol/L的范围内,荧光猝灭程度(F/F_(0))与Fe^(3+)浓度呈现良好的线性关系(R=0.9930),检测限为4.0μmol/L。同时探测温度对制备碳点的影响,在20-55℃范围内,碳点荧光强度与温度具有较好的线性响应。由于生理温度范围在此温度范围内,所制备的碳点可用于细胞温度传感。 展开更多
关键词 n s共掺杂碳点 微波法 fe^(3%PLUs%)检测 纳米温度计
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Highly efficient Fe/N/C catalyst using adenosine as C/N-source for APEFC
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作者 Huan Ren Ying Wang +3 位作者 Xun Tang Juntao Lu Li Xiao Lin Zhuang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第4期616-621,共6页
An environmentally friendly precursor, adenosine, has been used as a dual source of C and N to synthesize nitrogen-doped carbon catalyst with/without Fe. A hydrothermal carbonization method has been used and water is ... An environmentally friendly precursor, adenosine, has been used as a dual source of C and N to synthesize nitrogen-doped carbon catalyst with/without Fe. A hydrothermal carbonization method has been used and water is the carbonization media. The morphology of samples with/without Fe component has been compared by HRTEM, and the result shows that Fe can promote the graphitization of carbon. Further electro-chemical test shows that the oxygen reduction reaction(ORR) catalytic activity of Fe-containing sample(C–Fe N) is much higher than that of the Fe-free sample(C–N). Additionally, the intermediates of C–Fe N formed during each synthetic procedure have been thoroughly characterized by multiple methods,and the function of each procedure has been discussed. The C–Fe N sample exhibits high electro-catalytic stability and superior electro-catalytic activity toward ORR in alkaline media, with its half-wave potential 20 mV lower than that of commercial Pt/C(40 wt%). It is further incorporated into alkaline polymer electrolyte fuel cell(APEFC) as the cathode material and led to a power density of 100 m W/cm;. 展开更多
关键词 n-doped carbon catalyst ORR Fuel cell Alkaline polymer electrolyte fe/n/C
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Zn/Fe纳米颗粒共嵌入碳纳米管提高氧还原反应性能
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作者 吴梦雪 马金福 +4 位作者 刘子逸 刘慧泽 王冠东 陈轩毅 施志聪 《广东工业大学学报》 CAS 2023年第6期106-113,184,共9页
开发低成本、高稳定、高催化活性氧化还原反应(Oxygen Reduction Reaction,ORR)的非贵金属催化剂对燃料电池和金属-空气电池的应用至关重要。本文研究了以ZIF-8为前驱体一步合成ZnFe纳米颗粒嵌入N、S掺杂碳纳米管的复合催化剂(ZnS-FeS-F... 开发低成本、高稳定、高催化活性氧化还原反应(Oxygen Reduction Reaction,ORR)的非贵金属催化剂对燃料电池和金属-空气电池的应用至关重要。本文研究了以ZIF-8为前驱体一步合成ZnFe纳米颗粒嵌入N、S掺杂碳纳米管的复合催化剂(ZnS-FeS-Fe_(3)C/S,NCNT)。通过电化学测试确定最优煅烧温度后的样品ZFF/S,NCNT-8的起始电位Eo为0.99 V vs.RHE和半波电位E1/2为0.84 Vvs.RHE,并且与商业Pt/C相当,具有良好的甲醇耐受性和长期稳定性。同时也提出S、N共掺杂碳纳米管(Carbon Nanotube,CNT)和额外的ZnS、FeS和Fe_(3)提供活性位点可以提高ORR催化性能。文中所采用的原位生长CNT方法,可为制备燃料电池和金属-空气电池的阴极催化剂提供思路。 展开更多
关键词 氧还原反应 氮、硫掺杂碳纳米管 ZIF-8 热解 碳材料
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Edge-enriched N, S co-doped hierarchical porous carbon for oxygen reduction reaction
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作者 Fangfang Chang Panpan Su +5 位作者 Utsab Guharoy Runping Ye Yanfu Ma Huajun Zheng Yi Jia Jian Liu 《Chinese Chemical Letters》 SCIE CAS CSCD 2023年第2期349-354,共6页
The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the explorat... The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts. 展开更多
关键词 Porosity engineering n s co-doped carbon materials Hierarchical porous carbon Edge-enriched carbon Oxygen reduction reaction DFT calculation
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High N-doped hierarchical porous carbon networks with expanded interlayers for efficient sodium storage 被引量:11
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作者 Dongqin Su Man Huang +5 位作者 Junhao Zhang Xingmei Guo Jiale Chen Yanchun Xue Aihua Yuan Qinghong Kong 《Nano Research》 SCIE EI CAS CSCD 2020年第10期2862-2868,共7页
Sodium-ion batteries (SIBs) have been attracting considerable attention as a promising candidate for large-scale energy storage because of the abundance and low-cost of sodium resources. However, lack of appropriate a... Sodium-ion batteries (SIBs) have been attracting considerable attention as a promising candidate for large-scale energy storage because of the abundance and low-cost of sodium resources. However, lack of appropriate anode materials impedes further applications. Herein, a novel self-template strategy is designed to synthesize uniform flowerlike N-doped hierarchical porous carbon networks (NHPCN) with high content of N (15.31 at.%) assembled by ultrathin nanosheets via a self-synthesized single precursor and subsequent thermal annealing. Relying on the synergetic coordination of benzimidazole and 2-methylimidazole with metal ions to produce a flowerlike network, a self-formed single precursor can be harvested. Due to the structural and compositional advantages, including the high N doping, the expanded interlayer spacing, the ultrathin two-dimensional nano-sized subunits, and the three-dimensional porous network structure, these unique NHPCN flowers deliver ultrahigh reversible capacities of 453.7 mAh·g^−1 at 0.1 A·g^−1 and 242.5 mAh·g^−1 at 1 A·g^−1 for 2,500 cycles with exceptional rate capability of 5 A·g^−1 with reversible capacities of 201.2 mAh·g^−1. The greatly improved sodium storage performance of NHPCN confirms the importance of reasonable engineering and synthesis of hierarchical carbon with unique structures. 展开更多
关键词 hierarchical porous carbon networks high n doping expanded interlayer spacing AnODE sodium-ion batteries
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Fe/N共掺杂生物质活性炭提升氧化还原性能 被引量:1
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作者 王文泉 邢献军 +1 位作者 李珊 宋雨蔷 《真空科学与技术学报》 EI CAS CSCD 北大核心 2020年第3期273-279,共7页
以梧桐木屑为原料,采用湿混法与一定量KOH搅拌并干燥,在氮气氛围下高温活化制备生物质活性炭。选取工艺优化后的活性炭掺杂铁氮元素,二次高温煅烧后形成Fe-N-C型非贵重金属催化剂。得出木屑生物质活性炭在活化温度为800℃,碱料比1∶3下... 以梧桐木屑为原料,采用湿混法与一定量KOH搅拌并干燥,在氮气氛围下高温活化制备生物质活性炭。选取工艺优化后的活性炭掺杂铁氮元素,二次高温煅烧后形成Fe-N-C型非贵重金属催化剂。得出木屑生物质活性炭在活化温度为800℃,碱料比1∶3下比表面积为2051.8 m2·g-1,总孔容为1.23 cm3·g-1;通过进一步掺杂铁氮元素获得的催化剂材料拥有良好的ORR(氧还原反应)活性(初始电位-0.03 V、半波电位-0.10 V和极限电流4.2 mA/cm2)、耐甲醇性和稳定性,可以在能源领域中被广泛的应用。 展开更多
关键词 生物质活性碳 fe/n共掺杂 高比表面积 氧还原催化剂 梧桐木屑
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二维ZIF-L衍生的叶片状Fe-NC材料的制备及其氧还原催化性能研究 被引量:4
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作者 叶谢维伊 郑志平 匡勤 《无机盐工业》 CAS CSCD 北大核心 2021年第6期1-7,共7页
将柠檬酸铁铵作为Fe源掺入叶片状ZIF-L前驱体中,经过分段式高温热解成功制备出形貌维持良好的二维片状的Fe-NC催化剂。通过探究Fe载量对催化性质的影响发现,Fe-NC-1%催化剂在碱性电解质中呈现出最为优异的氧还原反应(ORR)活性,半波电位E... 将柠檬酸铁铵作为Fe源掺入叶片状ZIF-L前驱体中,经过分段式高温热解成功制备出形貌维持良好的二维片状的Fe-NC催化剂。通过探究Fe载量对催化性质的影响发现,Fe-NC-1%催化剂在碱性电解质中呈现出最为优异的氧还原反应(ORR)活性,半波电位E_(1/2)达到了0.897 V,动力学电流密度J0.85 V为26.70 mA/cm^(2),5000次循环过后E_(1/2)衰减5 mV,均超过了商业Pt/C催化剂。结合Raman光谱、XPS、BET法比表面积测定等分析表明,Fe-NC-1%的大比表面积、高石墨化程度、丰富的含氮活性物种等优势赋予了较高的传质效率及催化活性位点利用率,是促进其ORR反应动力学的重要因素。 展开更多
关键词 氧还原反应 ZIF-L 氮掺杂碳 铁基催化剂
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Effect of doping order on metal-free heteroatoms dual-doped carbon as oxygen reduction electrocatalyst
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作者 Hui-Juan Zhang Jing Geng +4 位作者 Chunlei Cai Zi-Feng Ma Zhong Ma Wenli Yao Junhe Yang 《Chinese Chemical Letters》 SCIE CAS CSCD 2021年第2期745-749,共5页
Metal-free heteroatoms dual-doped carbon has been recognized as one of the most promising Pt/C-substitutes for oxygen reduction reaction(ORR).Herein,we optimize the preparation process by doping order of metal-free he... Metal-free heteroatoms dual-doped carbon has been recognized as one of the most promising Pt/C-substitutes for oxygen reduction reaction(ORR).Herein,we optimize the preparation process by doping order of metal-free heteroatoms to obtain the best electrocatalytic performance through three types of dual-doped carbon,including XC-N(first X doping then N doping),NC-X(first N doping then X doping) and NXC(N and X doping)(X=P,S and F).XC-N has more defect than the other two indicated by Raman spectra.X-ray photoelectron spectrom(XPS) measurements indicate that N and X have been dual-doped into the carbon matrix with different doping contents and modes,Electrocatalytic results,including the potential of ORR peak(Ep),the half-wave potential,the diffusion-limiting current density mainly follows the order of XC-N>NC-X> NXC,Furthermore,the synergistic effect of second atom doping are also compared with the single doped carbon(NC,PC,SC and FC).The differences in electronegativity and atomic radius of these metal-free heteroatoms can affect the defect degree,the doping content and mode of hete roatoms on carbon matrix,induce polarization effect and space effect to affect O2 adsorption and product desorption,ultimately to the ORR electrocatalytic performance. 展开更多
关键词 Oxygen reduction reaction Metal-free electrocatalyst Heteroatoms dual-doped carbon Doping order n P s and F
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碳纳米管超晶格结构吸附Fe原子的电子机理 被引量:1
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作者 杨忠华 李荣德 曲迎东 《沈阳工业大学学报》 EI CAS 北大核心 2017年第4期383-388,共6页
为了提高碳纳米管与Fe基体之间的润湿性,构造出N掺杂有限长碳纳米管超晶格结构.第一性原理能量计算结果表明,新型超晶格结构的埋置能正向升高,结构稳定性降低,但可以显著提高外壁对Fe原子的吸附能力.差分电荷密度结果表明,掺杂体系中N... 为了提高碳纳米管与Fe基体之间的润湿性,构造出N掺杂有限长碳纳米管超晶格结构.第一性原理能量计算结果表明,新型超晶格结构的埋置能正向升高,结构稳定性降低,但可以显著提高外壁对Fe原子的吸附能力.差分电荷密度结果表明,掺杂体系中N原子与邻近C原子间的π键出现了畸变,使得N原子易与Fe原子发生结合.布居数和电荷转移情况表明,N原子的掺入导致Fe原子失电子能力降低,但Fe—N间共价键强度提高.超晶格结构在一定的扭转和剪切变形下仍能保持对Fe原子的吸附能力. 展开更多
关键词 碳纳米管 超晶格结构 n原子掺杂 fe原子吸附 电子机理 第一性原理 剪切变形 扭转变形
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N/S co-doped 3D carbon framework prepared by a facile morphology-controlled solid-state pyrolysis method for oxygen reduction reaction in both acidic and alkaline media 被引量:2
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作者 Juan Nong Min Zhu +4 位作者 Kun He Aosheng Zhu Pu Xie Minzhi Rong Mingqiu Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第7期220-226,共7页
Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only sh... Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium. 展开更多
关键词 3D n/s-doped carbon frameworks Oxygen reduction reaction(ORR) Morphology-retaining PYROLYsIs ACIDIC medium
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采用两步炭化法和熔盐模板法制备N、S共掺杂煤基硬炭及共储钠性能 被引量:1
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作者 牛慧祝 王海花 +6 位作者 孙立宇 杨晨榕 王雨 曹瑞 杨存国 王洁 舒珂维 《新型炭材料(中英文)》 SCIE EI CAS CSCD 北大核心 2024年第2期297-307,共11页
硬炭因资源丰富、结构稳定及安全性高等优势,已成为钠离子电池常用阳极材料。其中,煤基衍生硬炭受到了广泛的关注。本工作以长焰煤为碳源,硫脲为氮硫源,NaCl为模板,通过两步炭化工艺和杂原子掺杂相结合的方法合成了N和S共掺杂的煤基硬炭... 硬炭因资源丰富、结构稳定及安全性高等优势,已成为钠离子电池常用阳极材料。其中,煤基衍生硬炭受到了广泛的关注。本工作以长焰煤为碳源,硫脲为氮硫源,NaCl为模板,通过两步炭化工艺和杂原子掺杂相结合的方法合成了N和S共掺杂的煤基硬炭(NSPC1200)。两步炭化过程在调节碳微晶结构和扩大层间距方面发挥了重要的作用。N和S的共掺杂调节了炭材料的电子结构,赋予其更多的活性位点;此外,引入NaCl作为模板有助于孔结构的构建,有利于电极和电解质之间的接触,从而实现Na+和电子的有效传输。在协同作用下,样品NSPC1200表现出优异的储钠能力,在20 mA g^(−1)电流密度下呈现314.2 mAh g^(−1)的可逆容量。即使在100 mA g^(−1)下循环200次,仍保持224.4 mAh g^(−1)的比容量。这项工作成功实现了策略性调整煤基炭材料微观结构的目标,最终获得了具有优异的电化学性能的硬炭阳极。 展开更多
关键词 硬炭 钠离子电池 煤衍生炭 两步炭化 氮硫共掺杂
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