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Facile Ammonia Synthesis from Electrocatalytic N2 Reduction under Ambient Conditions on N-Doped Porous Carbon
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acscatal.7b02165 Yanming Liu 1 , Yan Su 2 , Xie Quan 1 , Xinfei Fan 1 , Shuo Chen 1 , Hongtao Yu 1 , Huimin Zhao 1 , Yaobin Zhang 1 , Jijun Zhao 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acscatal.7b02165 Yanming Liu 1 , Yan Su 2 , Xie Quan 1 , Xinfei Fan 1 , Shuo Chen 1 , Hongtao Yu 1 , Huimin Zhao 1 , Yaobin Zhang 1 , Jijun Zhao 2
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Ammonia has been used in important areas such as agriculture and clean energy. Its synthesis from the electrochemical reduction of N2 is an attractive alternative to the industrial method that requires high temperature and pressure. Currently, electrochemical N2 fixation has suffered from slow kinetics due to the difficulty of N2 adsorption and N≡N cleavage. Here, N-doped porous carbon (NPC) is reported as a cost-effective electrocatalyst for ammonia synthesis from electrocatalytic N2 reduction under ambient conditions, where its N content and species were tuned to enhance N2 chemical adsorption and N≡N cleavage. The resulting NPC was effective for fixing N2 to ammonia with a high ammonia production rate (1.40 mmol g–1 h–1 at −0.9 V vs RHE). Experiments combined with density functional theory calculations revealed pyridinic and pyrrolic N were active sites for ammonia synthesis and their contents were crucial for promoting ammonia production on NPC. The energy-favorable pathway for ammonia synthesis was *N≡N → *NH═NH → *NH2–NH2 → 2NH3.
中文翻译：
氮掺杂多孔碳在环境条件下电催化还原N 2合成氨
氨已用于农业和清洁能源等重要领域。由N 2的电化学还原合成的方法是需要高温和高压的工业方法的一种有吸引力的替代方法。目前，由于N 2吸附和N≡N裂解的困难，电化学N 2固定受到动力学的影响。在此，N掺杂多孔碳（NPC）被认为是在环境条件下通过电催化还原N 2来合成氨的一种经济高效的电催化剂，其氮含量和种类经过调整以增强N 2的化学吸附和N≡N裂解。所得的NPC对固定N 2有效。到具有高氨生产率的氨（在-0.9 V对RHE下为1.40 mmol g –1 h –1）。实验与密度泛函理论计算相结合，揭示了吡啶二氮和吡咯N是氨合成的活性位点，其含量对于促进NPC上氨的产生至关重要。氨合成的能量有利途径为*N≡N→*NH═NH→* NH 2 -NH 2 →2NH 3。
更新日期：2018-01-17
中文翻译：
氮掺杂多孔碳在环境条件下电催化还原N 2合成氨
氨已用于农业和清洁能源等重要领域。由N 2的电化学还原合成的方法是需要高温和高压的工业方法的一种有吸引力的替代方法。目前，由于N 2吸附和N≡N裂解的困难，电化学N 2固定受到动力学的影响。在此，N掺杂多孔碳（NPC）被认为是在环境条件下通过电催化还原N 2来合成氨的一种经济高效的电催化剂，其氮含量和种类经过调整以增强N 2的化学吸附和N≡N裂解。所得的NPC对固定N 2有效。到具有高氨生产率的氨（在-0.9 V对RHE下为1.40 mmol g –1 h –1）。实验与密度泛函理论计算相结合，揭示了吡啶二氮和吡咯N是氨合成的活性位点，其含量对于促进NPC上氨的产生至关重要。氨合成的能量有利途径为*N≡N→*NH═NH→* NH 2 -NH 2 →2NH 3。
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