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Single Ni atoms with higher positive charges induced by hydroxyls for electrocatalytic CO2 reduction.
Nanoscale ( IF 5.8 ) Pub Date : 2020-08-20 , DOI: 10.1039/d0nr04391e Xiao Yang 1 , Jun Cheng 1 , Baizeng Fang 2 , Xiaoxu Xuan 1 , Niu Liu 1 , Xian Yang 1 , Junhu Zhou 1
Nanoscale ( IF 5.8 ) Pub Date : 2020-08-20 , DOI: 10.1039/d0nr04391e Xiao Yang 1 , Jun Cheng 1 , Baizeng Fang 2 , Xiaoxu Xuan 1 , Niu Liu 1 , Xian Yang 1 , Junhu Zhou 1
Affiliation
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To promote the faradaic efficiency of the electrocatalytic CO2 reduction reaction (CO2RR) with low-cost catalysts, single Ni atoms with higher positive charges induced by hydroxyls were proposed to form an atomically dispersed Ni–N4 structure in a cheap honeycomb-like carbon matrix for electrocatalytic CO2 reduction. Extended X-ray absorption fine structure spectroscopy, aberration-corrected High-angle annular dark-field scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements confirmed that the active-center structure consists of single Ni atoms and the adjacent hydroxyl via hydrothermal treatment (H-Ni/NC). Density functional theory calculations indicated that the isolated Ni atoms with higher positive charges induced by the hydroxyl decreased the free energy of the rate-limiting step to 1.05 eV for the CO2RR. The faradaic efficiency (FE) of CO2 reduction into CO was ≥88.0% over the H-Ni/NC catalyst in the potential range of −0.5 to −0.9 V (vs. RHE). The peak CO FE reached 97% at −0.7 V due to the synergistic effect between the unsaturated Ni–N4 active sites and the hydroxyl species.
中文翻译：
羟基诱导的带有较高正电荷的单个Ni原子用于电催化还原CO2。
为了提高使用低成本催化剂进行电催化CO 2还原反应（CO 2 RR）的法拉第效率，提出了由羟基诱导的带有较高正电荷的单个Ni原子在便宜的蜂窝结构中形成原子分散的Ni–N 4结构。类似于碳基质，用于电催化还原CO 2。扩展X射线吸收精细结构谱，像差校正高角度环形暗场扫描透射电子显微镜和X射线光电子光谱测量证实，在有源中心结构由单一Ni原子和相邻的羟基通过水热处理（H-Ni / NC）。密度泛函理论计算表明，由羟基诱导的具有较高正电荷的离析的Ni原子将CO 2 RR限速步骤的自由能降低至1.05 eV 。在-0.5至-0.9 V的电位范围内（相对于RHE），在H-Ni / NC催化剂上，CO 2还原成CO的法拉第效率（FE）≥88.0％。由于不饱和Ni–N 4活性位与羟基物种之间的协同作用，在-0.7 V处，CO FE的峰值达到97％。
更新日期：2020-09-18
中文翻译：
羟基诱导的带有较高正电荷的单个Ni原子用于电催化还原CO2。
为了提高使用低成本催化剂进行电催化CO 2还原反应（CO 2 RR）的法拉第效率，提出了由羟基诱导的带有较高正电荷的单个Ni原子在便宜的蜂窝结构中形成原子分散的Ni–N 4结构。类似于碳基质，用于电催化还原CO 2。扩展X射线吸收精细结构谱，像差校正高角度环形暗场扫描透射电子显微镜和X射线光电子光谱测量证实，在有源中心结构由单一Ni原子和相邻的羟基通过水热处理（H-Ni / NC）。密度泛函理论计算表明，由羟基诱导的具有较高正电荷的离析的Ni原子将CO 2 RR限速步骤的自由能降低至1.05 eV 。在-0.5至-0.9 V的电位范围内（相对于RHE），在H-Ni / NC催化剂上，CO 2还原成CO的法拉第效率（FE）≥88.0％。由于不饱和Ni–N 4活性位与羟基物种之间的协同作用，在-0.7 V处，CO FE的峰值达到97％。
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