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Tailoring Oxygen Vacancies of BiVO4 toward Highly Efficient Noble‐Metal‐Free Electrocatalyst for Artificial N2 Fixation under Ambient Conditions
Small Methods ( IF 10.7 ) Pub Date : 2018-11-15 , DOI: 10.1002/smtd.201800333 Jia‐Xin Yao 1 , Di Bao 1, 2 , Qi Zhang 3 , Miao‐Miao Shi 1 , Yue Wang 1 , Rui Gao 1 , Jun‐Min Yan 1 , Qing Jiang 1
Small Methods ( IF 10.7 ) Pub Date : 2018-11-15 , DOI: 10.1002/smtd.201800333 Jia‐Xin Yao 1 , Di Bao 1, 2 , Qi Zhang 3 , Miao‐Miao Shi 1 , Yue Wang 1 , Rui Gao 1 , Jun‐Min Yan 1 , Qing Jiang 1
Affiliation
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Ammonia (NH3) is vital to human beings as an important energy carrier, fertilizer precursor, and fuel, while breakage of the NN bond in nitrogen (N2) is a kinetically complex and energetically challenging multistep reaction. Development of electrocatalysts for efficient NH3 electrosynthesis via the N2 reduction reaction (NRR) is highly desirable but remains a key challenge. In this work, based on the density functional theory calculations, a novel and effective strategy to boost the nitrogen electroreduction performance of BiVO4 by tailoring its oxygen vacancies (OVs) is first proposed and demonstrated. Unexpectedly, the noble‐metal‐free BiVO4 with the highest OVs concentration shows excellent NRR performances, including high NH3 yield rate (up to 8.60 µg h−1 mg−1cat.), high faradaic efficiency (10.04% at −0.5 V vs reversible hydrogen electrode), and good stability (up to 24 h) at ambient conditions, outperforming most reported NRR electrocatalysts under ambient conditions and even some under harsh conditions, which can be attributed to enhanced N2 adsorption energy and a more favorable active reaction site at the V atom with lower coordination and higher spin‐polarization with a localized magnetic moment due to the introduction of OVs.
中文翻译：
将BiVO4的氧空位量身定制为在环境条件下用于人工固氮的高效无贵金属电催化剂
氨（NH 3）作为重要的能量载体，肥料前体和燃料对人类至关重要，而氮（N 2）中NN键的断裂是动力学上复杂且在能量上具有挑战性的多步反应。经由N 2还原反应（NRR）开发用于有效NH 3电合成的电催化剂是非常需要的，但是仍然是关键的挑战。在这项工作中，基于密度泛函理论计算，首先提出并证明了通过调整BiVO 4的氧空位（OVs）来提高BiVO 4的氮电还原性能的新颖有效的策略。出乎意料的是，不含贵金属的BiVO 4最高OVs浓度显示出优异的NRR性能，包括高NH 3产率（高达8.60 µg h -1 mg -1 cat。），高法拉第效率（相对于可逆氢电极，在-0.5 V时为10.04％） （长达24小时）在环境条件下甚至在某些苛刻条件下的性能都优于大多数报道的NRR电催化剂，这可以归因于N 2吸附能的增强和在V原子上具有更佳的活性反应位点，且配位和催化活性较低。由于引入了OV，导致具有局部磁矩的更高的自旋极化。
更新日期：2018-11-15
中文翻译：
将BiVO4的氧空位量身定制为在环境条件下用于人工固氮的高效无贵金属电催化剂
氨（NH 3）作为重要的能量载体，肥料前体和燃料对人类至关重要，而氮（N 2）中NN键的断裂是动力学上复杂且在能量上具有挑战性的多步反应。经由N 2还原反应（NRR）开发用于有效NH 3电合成的电催化剂是非常需要的，但是仍然是关键的挑战。在这项工作中，基于密度泛函理论计算，首先提出并证明了通过调整BiVO 4的氧空位（OVs）来提高BiVO 4的氮电还原性能的新颖有效的策略。出乎意料的是，不含贵金属的BiVO 4最高OVs浓度显示出优异的NRR性能，包括高NH 3产率（高达8.60 µg h -1 mg -1 cat。），高法拉第效率（相对于可逆氢电极，在-0.5 V时为10.04％） （长达24小时）在环境条件下甚至在某些苛刻条件下的性能都优于大多数报道的NRR电催化剂，这可以归因于N 2吸附能的增强和在V原子上具有更佳的活性反应位点，且配位和催化活性较低。由于引入了OV，导致具有局部磁矩的更高的自旋极化。
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