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Two-Dimensional Mosaic Bismuth Nanosheets for Highly Selective Ambient Electrocatalytic Nitrogen Reduction
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-02-21 00:00:00 , DOI: 10.1021/acscatal.9b00366 Laiquan Li 1 , Cheng Tang 1 , Bingquan Xia 1 , Huanyu Jin 1 , Yao Zheng 1 , Shi-Zhang Qiao 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-02-21 00:00:00 , DOI: 10.1021/acscatal.9b00366 Laiquan Li 1 , Cheng Tang 1 , Bingquan Xia 1 , Huanyu Jin 1 , Yao Zheng 1 , Shi-Zhang Qiao 1
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Electrochemical fixation of N2 to ammonia is a promising strategy to store renewable energy and mitigate greenhouse gas emissions. However, it usually suffers from extremely low ammonia yield and Faradaic efficiency because of the lack of efficient electrocatalysts and the competing hydrogen evolution reaction. Herein, we report that the semiconducting bismuth can be a promising catalyst for ambient electrocatalytic N2 reduction reaction (NRR). A two-dimensional mosaic bismuth nanosheet (Bi NS) was fabricated via an in situ electrochemical reduction process and exhibited favorable average ammonia yield and Faradaic efficiency as high as 2.54 ± 0.16 μgNH3 cm–2 h–1 (∼13.23 μg mgcat.–1 h–1) and 10.46 ± 1.45% at −0.8 V versus reversible hydrogen electrode in 0.1 M Na2SO4. The high NRR electrocatalytic activity of the Bi NS could be attributed to the sufficient exposure of edge sites coupled with effective p-orbital electron delocalization in the mosaic bismuth nanosheets. In addition, the semiconducting feature, which limits surface electron accessibility, could effectively enhance the Faradaic efficiency. This work highlights the potential importance of less reactive main group elements with tunable p-electron density, semiconducting property, and ingenious nanostructure for further exploration of N2 reduction reaction electrocatalysts.
中文翻译：
二维马赛克式铋纳米片用于高选择性环境电催化氮还原
将N 2电化学固定为氨是存储可再生能源和减少温室气体排放的一种有前途的策略。然而，由于缺乏有效的电催化剂和竞争性的析氢反应，它通常遭受极低的氨产率和法拉第效率。在此，我们报道半导体铋可以作为环境电催化N 2还原反应（NRR）的有前途的催化剂。二维镶嵌铋纳米片的（Bi NS）中的溶液中原位电化学还原处理，通过制造和显示良好的平均氨产量和法拉第效率高达2.54±0.16微克NH 3厘米-2 ħ -1（~13.23微克毫克猫。–1 h –1）和-0.8 V时在0.1 M Na 2 SO 4中相对于可逆氢电极为10.46±1.45％。Bi NS的高NRR电催化活性可归因于镶嵌铋纳米片中边缘位点的充分暴露以及有效的p轨道电子离域。另外，限制表面电子可及性的半导体特性可以有效地提高法拉第效率。这项工作强调了具有可调p电子密度，半导体性质和巧妙纳米结构的反应性较低的主族元素对于进一步探索N 2还原反应电催化剂的潜在重要性。
更新日期：2019-02-21
中文翻译：
二维马赛克式铋纳米片用于高选择性环境电催化氮还原
将N 2电化学固定为氨是存储可再生能源和减少温室气体排放的一种有前途的策略。然而，由于缺乏有效的电催化剂和竞争性的析氢反应，它通常遭受极低的氨产率和法拉第效率。在此，我们报道半导体铋可以作为环境电催化N 2还原反应（NRR）的有前途的催化剂。二维镶嵌铋纳米片的（Bi NS）中的溶液中原位电化学还原处理，通过制造和显示良好的平均氨产量和法拉第效率高达2.54±0.16微克NH 3厘米-2 ħ -1（~13.23微克毫克猫。–1 h –1）和-0.8 V时在0.1 M Na 2 SO 4中相对于可逆氢电极为10.46±1.45％。Bi NS的高NRR电催化活性可归因于镶嵌铋纳米片中边缘位点的充分暴露以及有效的p轨道电子离域。另外，限制表面电子可及性的半导体特性可以有效地提高法拉第效率。这项工作强调了具有可调p电子密度，半导体性质和巧妙纳米结构的反应性较低的主族元素对于进一步探索N 2还原反应电催化剂的潜在重要性。
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