Han Qingxin, Lu Qiangqiang, Wang Xuechuan, Wei Chao, Guan Xiaoyu, Chen Luming, Wang Xiao, Li Ji
College of Bioresources Chemical and Materials Engineering, Shaanxi University of Science & Technology, Xi'an 710021, Shaanxi, China.
Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry, Ministry of Education & Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology, Shaanxi University of Science and Technology, Xi'an, 710021, China.
Mater Horiz. 2024 Jul 1;11(13):3166-3177. doi: 10.1039/d3mh01951a.
In the leather manufacturing industry, the management of substantial quantities of solid waste containing chrome shavings remains a formidable challenge. Concurrently, there is a pressing need for the development of pH-universal and economically viable electrocatalysts for the hydrogen evolution reaction (HER). In response to these intertwined challenges, this study proposes an innovative approach wherein the amino groups present on the surface of chrome shavings are utilized to immobilize single ruthenium atoms during pyrolysis, thereby facilitating the synthesis of hydrogen evolution electrocatalysts. The optimized sample, denoted as CN/CrO/Ru-1, demonstrates exceptional electrocatalytic performance, exhibiting an ultra-low overpotential of -28 mV in 1.0 M KOH at a current density of 10 mA cm, and it also exhibits good performance in acidic and neutral electrolytes. Importantly, these overpotentials surpass those reported for many previous ruthenium-based catalysts. Density functional theory (DFT) calculations elucidate that both oxygen (O) and chromium (Cr) moieties within CrO can engage in favorable interactions with the coordination patterns of the ruthenium (Ru) atoms, thereby elucidating the synergistic enhancement conferred by the chromium element in CN/CrO/Ru, which ultimately facilitates and promotes the catalytic activity of the ruthenium atoms serving as the catalytic center. This facile synthesis route not only presents a green solution for addressing waste chromium pollutants but also offers a promising avenue for the development of high-performance, cost-efficient electrocatalysts.
在皮革制造行业，管理大量含铬刨花的固体废物仍然是一项艰巨的挑战。与此同时，迫切需要开发用于析氢反应（HER）的pH通用且经济可行的电催化剂。针对这些相互交织的挑战，本研究提出了一种创新方法，即在热解过程中利用铬刨花表面存在的氨基固定单个钌原子，从而促进析氢电催化剂的合成。优化后的样品标记为CN/CrO/Ru-1，表现出优异的电催化性能，在1.0 M KOH中，电流密度为10 mA cm时，具有-28 mV的超低过电位，并且在酸性和中性电解质中也表现出良好的性能。重要的是，这些过电位超过了许多先前报道的钌基催化剂的过电位。密度泛函理论（DFT）计算表明，CrO中的氧（O）和铬（Cr）部分都可以与钌（Ru）原子的配位模式发生有利的相互作用，从而阐明了CN/CrO/Ru中铬元素赋予的协同增强作用，这最终促进并提升了作为催化中心的钌原子的催化活性。这种简便的合成路线不仅为解决含铬废物污染物提供了一种绿色解决方案，还为开发高性能、低成本的电催化剂提供了一条有前景的途径。
