Molten NaCl-Assisted Synthesis of Porous Fe-N-C Electrocatalysts with a High Density of Catalytically Accessible FeN_4 Active Sites and Outstanding Oxygen Reduction Reaction Performance

Wang Qing; Yang Yuqi; Sun Fanfei; Chen Guangbo; Wang Jian; Peng Lishan; Chen Wan-Ting; Shang Lu; Zhao Jiaqi; Sun-Waterhouse Dongxiao; Zhang Tierui; Waterhouse Geoffrey I. N.

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Molten NaCl-Assisted Synthesis of Porous Fe-N-C Electrocatalysts with a High Density of Catalytically Accessible FeN_4 Active Sites and Outstanding Oxygen Reduction Reaction Performance

机译：熔融NaCl辅助合成多孔Fe-N-C电催化剂，具有高密度的催化途径Fen_4活性位点和出色的氧还原反应性能

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Iron single atom catalysts (FeN4) hosted in the micropores of N-doped carbons offer excellent performance for the oxygen reduction reaction (ORR). Achieving a high density of FeN4 sites accessible for ORR has proved challenging to date. Herein, a simple surface NaCl-assisted method towards microporous N-doped carbon electrocatalysts with an abundance of catalytically accessible FeN4 sites is reported. Powder mixtures of microporous zeolitic imidazolate framework-8 and NaCl are first heated to 1000 degrees C in N-2, with the melting of NaCl above 800 degrees C creating a highly porous N-doped carbon product (NC-NaCl). Ferric (Fe3+) ions are then adsorbed onto NC-NaCl, with a second pyrolysis stage at 900 degrees C in N-2 yielding a porous Fe/NC-NaCl electrocatalyst (Brunauer-Emmett-Teller surface area, 1911 m(2) g(-1)) with an excellent dispersion and high density of accessible surface FeN4 sites (26.3 x 10(19) sites g(-1)). The Fe/NC-NaCl electrocatalyst exhibits outstanding ORR performance with a high half-wave potential of 0.832 V (vs reversible hydrogen electrode) in 0.1 m HClO4. When used as the ORR cathode catalyst in a 1.0 bar H-2-O-2 fuel cell, Fe/NC-NaCl offers a high peak power density of 0.89 W cm(-2), ranking it as one of the most active M-N-C materials reported to date.

机译：在N掺杂碳的微孔中载有铁的铁单原子催化剂（FEN4）为氧还原反应（ORR）提供了出色的性能。迄今为止，可以获得挑战的ORR可访问的高密度的FEN4网站。这里，报道了一种简单的表面NaCl辅助方法，朝向微孔N掺杂的碳电催化剂具有丰富的催化易于的FEN4位点。微孔沸石咪唑酯框架-8和NaCl的粉末混合物首先在N-2中加热至1000℃，熔化NaCl以上800℃，产生高度多孔的N掺杂碳产物（NC-NaCl）。然后将铁（Fe 3 +）离子吸附在Nc-NaCl上，在900摄氏度下在N-2中具有第二热解阶段，得到多孔Fe / NC-NaCl电催化剂（Brunauer-Emmett-Teller表面积，1911 m（2）G （-1））具有优异的分散和高密度的可接近表面FEN4位点（26.3×10（19）位G（-1））。 Fe / NC-NaCl电催化剂表现出优异的ORR性能，在0.1M HClO4中具有0.832V（Vs可逆氢电极）的高半波电位。当用作1.0巴H-2-O-2燃料电池中的ORR阴极催化剂时，Fe / NC-NaCl提供0.89W厘米（-2）的高峰功率密度，将其排名为最活跃的MNC之一迄今为止报告的材料。

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来源
《Advanced energy materials》 |2021年第19期|2100219.1-2100219.9|共9页
作者
Wang Qing; Yang Yuqi; Sun Fanfei; Chen Guangbo; Wang Jian; Peng Lishan; Chen Wan-Ting; Shang Lu; Zhao Jiaqi; Sun-Waterhouse Dongxiao; Zhang Tierui; Waterhouse Geoffrey I. N.;
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作者单位

Univ Auckland Sch Chem Sci Auckland 1142 New Zealand;

Chinese Acad Sci Shanghai Synchrotron Radiat Facil Shanghai Inst Appl Phys Shanghai 201204 Peoples R China;

Chinese Acad Sci Shanghai Synchrotron Radiat Facil Shanghai Inst Appl Phys Shanghai 201204 Peoples R China;

Chinese Acad Sci Key Lab Photochem Convers & Optoelect Mat Tech Inst Phys & Chem Beijing 100190 Peoples R China;

Chongqing Univ Sch Chem & Chem Engn Chongqing Key Lab Chem Proc Clean Energy & Resour Chongqing 400030 Peoples R China;

Univ Auckland Sch Chem Sci Auckland 1142 New Zealand;

Univ Auckland Sch Chem Sci Auckland 1142 New Zealand;

Chinese Acad Sci Key Lab Photochem Convers & Optoelect Mat Tech Inst Phys & Chem Beijing 100190 Peoples R China;

Chinese Acad Sci Key Lab Photochem Convers & Optoelect Mat Tech Inst Phys & Chem Beijing 100190 Peoples R China;

Univ Auckland Sch Chem Sci Auckland 1142 New Zealand;

Chinese Acad Sci Key Lab Photochem Convers & Optoelect Mat Tech Inst Phys & Chem Beijing 100190 Peoples R China;

Univ Auckland Sch Chem Sci Auckland 1142 New Zealand;

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正文语种 eng
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关键词
Fe#8208; N#8208; C; oxygen reduction reaction; proton exchange membrane fuel cells; surface etching; utilization of FeN; (4) sites;

机译：Fe＆＃8208;n＆＃8208;c;氧还原反应;质子交换膜燃料电池;表面蚀刻;使用fen;（4）位点;

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1. Zinc-Mediated Template Synthesis of Fe-N-C Electrocatalysts with Densely Accessible Fe-N_x Active Sites for Efficient Oxygen Reduction [J] . Chen Guangbo, Liu Pan, Liao Zhongquan, Advanced Materials . 2020,第8期

机译：锌介导的Fe-N-x电催化剂的模板合成，该催化剂具有大量可访问的Fe-N_x活性位，可有效减少氧气
2. Facile enhancement of the active catalytic sites of N-doped graphene as a high performance metal-free electrocatalyst for oxygen reduction reaction [J] . Rahsepar Mansour, Nobakht Mohammad Reza, Kim Hasuck, Applied Surface Science . 2018,第JULa31期

机译：方便地增强N掺杂石墨烯的活性催化位点，作为用于氧还原反应的高性能无金属电催化剂
3. Air plasma etching towards rich active sites in Fe/N-porous carbon for the oxygen reduction reaction with superior catalytic performance [J] . Zhong Wenhua, Chen Jiaxiang, Zhang Peixin, Journal of Materials Chemistry, A. Materials for energy and sustainability . 2017,第32期

机译：空气等离子体蚀刻Fe / N-多孔碳中的富活性位点，用于氧还原反应，具有优异的催化性能
4. PANI-derived 3D hierarchical porous urchin-like Fe-N-C nanostructures as an outstanding electrocatalysts for the oxygen reduction reaction [C] . M.J. Park, S.J. Yoo, J.H. Jang World Hydrogen Energy Conference . 2017

机译：PANI-衍生的3D层次多孔核素样Fe-N-C纳米结构作为氧还原反应的出色电催化剂
5. Catalytic Activity and Durability of Non-Carbon Supported Platinum Electrocatalysts for Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells Environment [D] . Mirshekari, Gholamreza. 2018

机译：质子交换膜燃料电池环境中非碳载铂电催化剂对氧还原反应的催化活性和耐久性
6. Shape controlled synthesis of porous tetrametallic PtAgBiCo nanoplates as highly active and methanol-tolerant electrocatalyst for oxygen reduction reaction [O] . Azhar Mahmood, Nanhong Xie, Muhammad Aizaz Ud Din, 2017

机译：形状控制合成多孔四金属PtAgBiCo纳米板作为高活性和耐甲醇的氧还原反应电催化剂
7. Effects of the induced micro- and meso-porosity on the single site density and turn over frequency of Fe-N-C carbon electrodes for the oxygen reduction reaction [O] . Marco Mazzucato, Giorgia Daniel, Asad Mehmood, 2021

机译：诱导的微孔和中孔孔对单位密度对Fe-N-C碳电极转动氧还原反应的影响

Molten NaCl-Assisted Synthesis of Porous Fe-N-C Electrocatalysts with a High Density of Catalytically Accessible FeN_4 Active Sites and Outstanding Oxygen Reduction Reaction Performance

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