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PEO-b-PS Block Copolymer Templated Mesoporous Carbons: A Comparative Study of Nitrogen and Sulfur Doping in the Oxygen Reduction Reaction to Hydrogen Peroxide.
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2020-09-21 , DOI: 10.1002/chem.202003355 Valentina Perazzolo 1 , Giorgia Daniel 1 , Riccardo Brandiele 1 , Luca Picelli 1 , Gian Andrea Rizzi 1 , Abdirisak Ahmed Isse 1 , Christian Durante 1
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2020-09-21 , DOI: 10.1002/chem.202003355 Valentina Perazzolo 1 , Giorgia Daniel 1 , Riccardo Brandiele 1 , Luca Picelli 1 , Gian Andrea Rizzi 1 , Abdirisak Ahmed Isse 1 , Christian Durante 1
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Carbon materials slightly doped with heteroatoms such as nitrogen (N‐RFC) or sulfur (S‐RFC) are investigated as active catalysts for the electrochemical bielectronic oxygen reduction reaction (ORR) to H2O2. Mesoporous carbons with wide, accessible pores were prepared by pyrolysis of a resorcinol‐formaldehyde resin using a PEO‐b‐PS block copolymer as a sacrificial templating agent and the nitrogen and sulfur doping were accomplished in a second thermal treatment employing 1,10‐phenanthroline and dibenzothiophene as nitrogen and sulfur precursors, respectively. The synthetic strategy allowed to obtain carbon materials with very high surface area and mesopore volume without any further physicochemical post treatment. Voltammetric rotating ring‐disk measurements in combination with potentiostatic and galvanostatic bulk electrolysis measurements in 0.5 m H2SO4 demonstrated a pronounced effect of heteroatom doping and mesopores volume on the catalytic activity and selectivity for H2O2. N‐RFC electrode was employed as electrode material in a 45 h electrolysis showing a constant H2O2 production of 298 mmol g−1 h−1 (millimoles of H2O2 divided by mass of catalyst and electrolysis time), with a faradic efficiency (FE) up to 61 % and without any clear evidence of degradation. The undoped carbon RFC showed a lower production rate (218 mmol g−1 h−1) but a higher FE of 76 %, while the performances drastically dropped when S‐RFC (production rate 11 mmol g−1 h−1 and FE=39 %) was used.
中文翻译：
PEO-b-PS嵌段共聚物模板化的介孔碳：氮和硫掺杂过氧化氢的氧还原反应中的比较研究。
略微掺杂有杂原子如氮（N-RFC）或硫（S-RFC）的碳材料进行了研究作为活性催化剂用于电化学bielectronic氧还原反应（ORR）至H 2 ö 2。通过使用PEO-b-PS嵌段共聚物作为牺牲模板剂对间苯二酚-甲醛树脂进行热解制备具有宽大可及孔的介孔碳，并在第二次热处理中使用1,10-菲咯啉掺杂氮和硫和二苯并噻吩分别作为氮和硫的前体。合成策略允许获得具有非常高的表面积和中孔体积的碳材料，而无需任何进一步的物理化学后处理。伏安旋转圆盘测量与恒电位和恒电流本体电解测量相结合，在0.5 m H 2 SO 4中证明杂原子掺杂和中孔体积对H 2 O 2的催化活性和选择性有明显的影响。N-RFC电极在45 h电解中用作电极材料，显示出恒定的H 2 O 2产生298 mmol g -1 h -1（H 2 O 2的毫摩尔除以催化剂的质量和电解时间），且法拉第效率（FE）高达61％，并且没有任何明显的降解迹象。未掺杂碳RFC显示出较低的生产率（218 mmol g -1 h -1），但FE高达76％，而使用S‐RFC（生产率11 mmol g -1 h -1且FE = 39％）时性能急剧下降。
更新日期：2020-09-21
中文翻译：
PEO-b-PS嵌段共聚物模板化的介孔碳：氮和硫掺杂过氧化氢的氧还原反应中的比较研究。
略微掺杂有杂原子如氮（N-RFC）或硫（S-RFC）的碳材料进行了研究作为活性催化剂用于电化学bielectronic氧还原反应（ORR）至H 2 ö 2。通过使用PEO-b-PS嵌段共聚物作为牺牲模板剂对间苯二酚-甲醛树脂进行热解制备具有宽大可及孔的介孔碳，并在第二次热处理中使用1,10-菲咯啉掺杂氮和硫和二苯并噻吩分别作为氮和硫的前体。合成策略允许获得具有非常高的表面积和中孔体积的碳材料，而无需任何进一步的物理化学后处理。伏安旋转圆盘测量与恒电位和恒电流本体电解测量相结合，在0.5 m H 2 SO 4中证明杂原子掺杂和中孔体积对H 2 O 2的催化活性和选择性有明显的影响。N-RFC电极在45 h电解中用作电极材料，显示出恒定的H 2 O 2产生298 mmol g -1 h -1（H 2 O 2的毫摩尔除以催化剂的质量和电解时间），且法拉第效率（FE）高达61％，并且没有任何明显的降解迹象。未掺杂碳RFC显示出较低的生产率（218 mmol g -1 h -1），但FE高达76％，而使用S‐RFC（生产率11 mmol g -1 h -1且FE = 39％）时性能急剧下降。
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