通过操纵单个原子的第二协调来优化中间体吸附,以有效地氧化水
1Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
调节单原子催化剂 (SAC) 的协调环境是性能的关键. 在Ir1-NiO中适度的协调通过优化中间结合来增强氧演变反应 (OER) 活性.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 表面化学 表面化学
背景情况:
- 对单原子催化剂 (SAC) 当地化学环境的精确控制对于理解结构-活性关系至关重要.
- 第二个协调外对SAC性能的影响是复杂的,需要进一步研究,特别是对于氧化物支持系统.
- 在坚固的氧化物支上操纵单个原子的第二个协调外是一个重要的合成挑战.
研究的目的:
- 调查第二协调变化的影响,以氧化 (NiO) 支持的单原子催化剂 (SACs) 的催化性能.
- 为了确定Ir-O-Ni协调数与氧演化反应 (OER) 的活性之间的相关性.
主要方法:
- 三种不同的单原子催化剂 (SAC) 的合成:Ir1/NiO,Ir1-NiO和Ir1@NiO,具有增加的Ir-O-Ni协调数 (3,4和5分别).
- 电化学表征以评估合成的SACs的氧化演化反应 (OER) 性能.
- 在现场进行机械研究,以阐明电子结构和中间吸附特性.
主要成果:
- 合成的SACs的OER活动表现出与Ir-O-Ni协调号有关的火山形趋势.
- 具有4的适度Ir-O-Ni协调数的Ir1-NiO表现出最高的OER活性,在10mA cm-2.2时达到225mV的低超电位.
- 机械研究表明,Ir1-NiO中适度的协调优化了Ir d<0xE1><0xB5><0xA3>2轨道占用率,削弱了*OOH中间吸附,提高了OER效率.
结论:
- 第二个协调在调整单原子催化剂的催化活性方面发挥着至关重要的作用.
- 适度的Ir-O-Ni协调是优于提高氧演化反应 (OER) 在NiO上的基于Ir的SAC中的性能.
- 了解和控制本地协调环境是设计高效电催化剂的可行策略.
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