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C2N-graphene supported single-atom catalysts for CO2 electrochemical reduction reaction: mechanistic insight and catalyst screening†
Nanoscale ( IF 5.8 ) Pub Date : 2018-07-20 00:00:00 , DOI: 10.1039/c8nr04961k Xudong Cui 1, 2, 3, 4 , Wei An 1, 2, 3, 4 , Xiaoyang Liu 1, 2, 3, 4 , Hao Wang 1, 2, 3, 4 , Yong Men 1, 2, 3, 4 , Jinguo Wang 1, 2, 3, 4
Nanoscale ( IF 5.8 ) Pub Date : 2018-07-20 00:00:00 , DOI: 10.1039/c8nr04961k Xudong Cui 1, 2, 3, 4 , Wei An 1, 2, 3, 4 , Xiaoyang Liu 1, 2, 3, 4 , Hao Wang 1, 2, 3, 4 , Yong Men 1, 2, 3, 4 , Jinguo Wang 1, 2, 3, 4
Affiliation
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Single-atom catalysts (SACs) have emerged as an excellent platform for enhancing catalytic performance. Inspired by the recent experimental synthesis of nitrogenated holey 2D graphene (C2N-h2D) (Mahmood et al., Nat. Commun., 2015, 6, 6486–6493), we report density functional theory calculations combined with computational hydrogen electrode model to show that C2N-h2D supported metal single atoms (M@C2N) are promising electrocatalysts for CO2 reduction reaction (CO2 RR). M confined at pyridinic N6 cavity promotes activation of inert O![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
CO bonds and subsequent protonation steps, with *COOH → *CO → CHO predicted to be the primary pathway for producing methanol and methane. It is found that *CO + H+ + e− → *CHO is most likely to be the potential determining step; breaking the scaling relation of *CO and *CHO binding on M@C2N SACs may simply be a rare event that is sensitively controlled by the detailed geometry of the adsorbate. Among twelve metals screened, M@C2N SACs where M = Ti, Mn, Fe, Co, Ni, Ru were identified to be effective in catalyzing CO2 RR with lowered overpotentials (0.58 V–0.80 V).
中文翻译：
用于CO 2电化学还原反应的 C 2 N-石墨烯负载单原子催化剂：机理见解和催化剂筛选†
单原子催化剂（SAC）已经成为增强催化性能的绝佳平台。由最近的氮化多孔2D石墨烯的实验合成（C启发2的N- H2D）（马哈茂德等人，纳特。COMMUN。，2015，6，6486-6493），我们报告密度泛函理论计算与计算氢电极模型结合表明C 2 N-h2D负载的金属单原子（M @ C 2 N）是用于CO 2还原反应（CO 2 RR）的有前途的电催化剂。限制在吡啶N6腔中的M促进了惰性OC的活化O键和随后的质子化步骤，其中* COOH→* CO→CHO被预测为生产甲醇和甲烷的主要途径。据发现，* CO + H + + E - →* CHO是最有可能被确定步骤的可能性; 打破在M @ C 2 N SAC上* CO和* CHO结合的比例关系可能只是罕见的事件，受吸附物的详细几何形状敏感地控制。在筛选出的十二种金属中，M @ C 2 N SACs（其中M = Ti，Mn，Fe，Co，Ni，Ru）被认为可有效地以较低的过电势（0.58 V–0.80 V）催化CO 2 RR。
更新日期：2018-07-20
CO bonds and subsequent protonation steps, with *COOH → *CO → CHO predicted to be the primary pathway for producing methanol and methane. It is found that *CO + H+ + e− → *CHO is most likely to be the potential determining step; breaking the scaling relation of *CO and *CHO binding on M@C2N SACs may simply be a rare event that is sensitively controlled by the detailed geometry of the adsorbate. Among twelve metals screened, M@C2N SACs where M = Ti, Mn, Fe, Co, Ni, Ru were identified to be effective in catalyzing CO2 RR with lowered overpotentials (0.58 V–0.80 V).
中文翻译：
用于CO 2电化学还原反应的 C 2 N-石墨烯负载单原子催化剂：机理见解和催化剂筛选†
单原子催化剂（SAC）已经成为增强催化性能的绝佳平台。由最近的氮化多孔2D石墨烯的实验合成（C启发2的N- H2D）（马哈茂德等人，纳特。COMMUN。，2015，6，6486-6493），我们报告密度泛函理论计算与计算氢电极模型结合表明C 2 N-h2D负载的金属单原子（M @ C 2 N）是用于CO 2还原反应（CO 2 RR）的有前途的电催化剂。限制在吡啶N6腔中的M促进了惰性O
C的活化O键和随后的质子化步骤，其中* COOH→* CO→CHO被预测为生产甲醇和甲烷的主要途径。据发现，* CO + H + + E - →* CHO是最有可能被确定步骤的可能性; 打破在M @ C 2 N SAC上* CO和* CHO结合的比例关系可能只是罕见的事件，受吸附物的详细几何形状敏感地控制。在筛选出的十二种金属中，M @ C 2 N SACs（其中M = Ti，Mn，Fe，Co，Ni，Ru）被认为可有效地以较低的过电势（0.58 V–0.80 V）催化CO 2 RR。
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