氮掺杂碳原位锚定铜纳米颗粒用于高效氧还原反应催化剂 |
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引用本文: | 袁会芳,张越,翟兴吾,胡立兵,葛桂贤,王刚,于锋,代斌.氮掺杂碳原位锚定铜纳米颗粒用于高效氧还原反应催化剂[J].电化学,2021,27(6):671. |
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作者姓名: | 袁会芳 张越 翟兴吾 胡立兵 葛桂贤 王刚 于锋 代斌 |
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作者单位: | 1.石河子大学化学化工学院,新疆兵团绿色化工过程重点实验室,新疆 石河子 8320032.石河子大学理学院,新疆 石河子 8320033.石河子大学兵团工业技术研究院,清洁能源转化与储存研究组,新疆 石河子 832003 |
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基金项目: | 国家自然科学基金项目(21865025);国家自然科学基金项目(51962032) |
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摘 要: | 与贵金属铂基电化学氧还原反应(ORR)催化剂相比,廉价的非贵金属催化剂引起了广泛的关注。本文以壳聚糖作为一种富含氮和碳元素的生物质资源,利用碳浴法成功制备了氮掺杂碳原位负载铜纳米颗粒(Cu/N-C)催化剂。纯壳聚糖碳化得到的样品N-C的比表面积为67.5 m2·g-1、平均孔径0.14 nm、平均孔体积8.00 m2·g-1,与之相比,Cu/N-C比表面积可达607.3 m2·g-1、平均孔径为2.5 nm、平均孔体积为0.40 cm3·g-1。通过密度泛函理论(DFT)进行计算表明,Cu(111)/N-C的自由能值低于N-C,更有利于氧还原催化进行。在0.1 mol·L-1 KOH的介质中,Cu/N-C不仅表现出优异的起始和半波电势(分别为0.96 V和0.84 V),而且还表现出了优异的抗甲醇性能和稳定性,并且Cu元素掺杂量达到1.67wt.%。
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关 键 词: | Cu/N-C 壳聚糖 生物质资源 催化剂 氧还原反应 碳浴法 |
收稿时间: | 2020-07-24 |
Copper Nanoparticles In-Situ Anchored on Nitrogen-Doped Carbon for High-Efficiency Oxygen Reduction Reaction Electrocatalyst |
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Abstract: | Compared with noble metal platinum (Pt)-based catalysts, inexpensive non-noble metal electrocatalysts have attracted extensive attention for oxygen reduction reaction (ORR). Herein, chitosan as a kind of biomass resource rich in nitrogen and carbon was used to prepare nitrogen-doped carbon (N-C) and N-C in-situ anchored by copper nanoparticles (Cu/N-C). The as-obtained N-C and Cu/N-C nanoparticles were successfully used as non-noble eletrocatalysts tested for ORR. Compared with the N-C, the Cu/N-C showed the high surface area of 607.3 m 2·g-1 with the mean pore size of 2.5 nm and the pore volume of 0.40 cm3·g-1. The most positive Gibbs free energy change was the rate determining step for ORR process with the 4e mechanism, where the value of the Cu(111)/N-C(-0.39 eV) was lower than that of the N-C(-0.26 eV). The Cu/N-C exhibited superior onset and half-wave potentials (0.96 V and 0.84 V, respectively) in alkaline media(0.1 mol·L-1 KOH), all of which are much better than those measured for N-C and commercial Pt/C. Furthermore, the Cu/N-C showed superior methanol crossover avoidance and oxygen reduction stability. |
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Keywords: | Cu/N-C chitosan biomass resource electrochemical catalyst oxygen reduction reaction carbon-bath method |
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