Hu Kui, Zhang Shengbo, Mao Zhixian, Zhao Dongnan, Li Daopeng, Li Zhongjun, Li Qiang, Tang Qiong, Shi Tongfei
School of Physics, Hefei University of Technology Hefei 230009 Anhui China
Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences Hefei 230031 China
RSC Adv. 2025 May 7;15(19):14739-14744. doi: 10.1039/d5ra00886g. eCollection 2025 May 6.
Ammonia (NH) is an important energy carrier and agricultural fertilizer. Development of electrocatalysts for efficient NH electrosynthesis the nitrate reduction reaction (NitRR) is highly desirable but remains a key challenge. In this work, we successfully loaded Au nanoparticles on BiVO by a one-step hydrothermal method. It is demonstrated that by using Au nanoparticles (10-15 nm) embedded on BiVO (Au/BiVO) with oxygen vacancies (Au loading is 1.3 wt%), the electrocatalytic NitRR is indeed possible under ambient conditions. Unexpectedly, at -1.35 V ( RHE), the yield rate for NH of Au/BiVO reached 3320.9 ± 89.9 μg h cm, which was far superior to (11.3 μg h cm) pristine BiVO. The N isotope labeling experiments confirmed that the produced NH indeed originated from the nitrate reduction reaction catalyzed by Au/BiVO. The comprehensive analysis further confirms that the oxygen vacancies in Au/BiVO can effectively weaken the N-O bonding and restrain the formation of by-products, resulting in high faradaic efficiency and NH selectivity. Furthermore, differential electrochemical mass spectrometry (DEMS) was adopted to monitor the electrochemical separation of the NitRR products on the surface of Au/BiVO.
氨（NH₃）是一种重要的能量载体和农业肥料。开发用于高效氨电合成即硝酸盐还原反应（NitRR）的电催化剂是非常有必要的，但仍然是一项关键挑战。在这项工作中，我们通过一步水热法成功地将金纳米颗粒负载在BiVO₄上。结果表明，通过使用嵌入在具有氧空位的BiVO₄上的金纳米颗粒（10 - 15纳米）（金负载量为1.3 wt%），在环境条件下电催化NitRR确实是可行的。出乎意料的是，在 - 1.35 V（相对于可逆氢电极）时，Au/BiVO₄的NH₃产率达到3320.9 ± 89.9 μg h⁻¹ cm⁻²，远优于原始BiVO₄（11.3 μg h⁻¹ cm⁻²）。氮同位素标记实验证实，产生的NH₃确实源自Au/BiVO₄催化的硝酸盐还原反应。综合分析进一步证实，Au/BiVO₄中的氧空位可以有效削弱N - O键并抑制副产物的形成，从而导致高法拉第效率和NH₃选择性。此外，采用差分电化学质谱（DEMS）来监测Au/BiVO₄表面上NitRR产物的电化学分离。
