High mass-specific reactivity of a defect-enriched Ru electrocatalyst for hydrogen evolution in harsh alkaline and acidic media
High mass-specific reactivity of a defect-enriched Ru electrocatalyst for hydrogen evolution in harsh alkaline and acidic media
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DOI：
10.1007/s40843-020-1656-0
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发表时间：
2021-04-29
影响因子：
8.1
通讯作者：
Liu, Qinghua
中科院分区：
文献类型：
--
作者：
Li, Yuanli;He, Jingfu;Liu, Qinghua
采用合理的设计策略，提高贵金属电催化剂在析氢反应(HER)中的利用率，是简化工艺流程、促进未来可再生能源经济的关键。在这里，在2.4 nm的Ru纳米粒子上产生了大量的缺陷，以在苛刻的酸性和碱性电解液中实现前所未有的高质量比反应性。得到的富缺陷Ru(DR-Ru)在碱性介质中表现出超高的Her转换频率16.4Her-S(-1)和100 mV的过电势，在酸性介质中也保持了20.6 S(-1)的优异的值，这些结果优于已报道的Ru催化剂。因此，在碱性和酸性介质中，DR-Ru催化剂的负载量为2.5微克厘米(-2)，在10 mA cm(-2)时的过电位分别为28.2 mV和25.1 mV。此外，较少配位的Ru表面位置和部分晶格氧的引入削弱了H和DR-Ru催化剂之间的成键，促进了快速酸性HER动力学，并帮助解离了水分子，克服了HER在碱性电解液中的主要挑战，导致了与酸性条件下相当的活性。这一结果为贵金属纳米催化剂的缺陷工程提供了指导，从而有效地提高了催化剂的利用率，优化了反应活性。
A reasonable design strategy to improve the utilization of noble metal electrocatalysts for the hydrogen evolution reaction (HER) is crucial to simplify the process flow and accelerate the future renewable energy economy. Here, abundant defects were created on 2.4-nm Ru nanoparticles to achieve unprecedently high mass-specific reactivity in harsh acidic and alkaline electrolytes. The obtained defect-enriched Ru (DR-Ru) exhibits an ultrahigh HER turnover frequency of 16.4 s(-1) with a 100-mV overpotential in alkaline media, and it also retains an excellent value of 20.6 s(-1) in acidic media; these results are superior to those reported for other Ru catalysts. Accordingly, a record-low loading of 2.5 mu g cm(-2) for the DR-Ru catalysts and low overpotentials of 28.2 and 25.1 mV at 10 mA cm(-2) can be realized in alkaline and acidic media, respectively. Furthermore, the less coordinated Ru surface sites and partial lattice oxygen introduction weaken the bonding between H and DR-Ru catalysts, facilitate fast acidic HER kinetics and help dissociate the water molecule to overcome the major challenge of HER in alkaline electrolytes, leading to an activity comparable to that under acidic conditions. This result provides a guideline for defect engineering on noble metal nanocatalysts to effectively improve the utilization of the catalysts and optimize reactivities.