Zhao Bin, Liu Jianwen, Feng Renfei, Wang Lei, Zhang Jiujun, Luo Jing-Li, Fu Xian-Zhu
Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060, China.
Canadian Light Source Inc., Saskatoon, Saskatchewan, S7N 0X4, Canada.
Small Methods. 2022 Mar;6(3):e2101195. doi: 10.1002/smtd.202101195. Epub 2021 Dec 19.
Energy crises, environmental pollution, and freshwater deficiency are critical issues on the planet. Electrolytic hydrogen generation from saline water, particularly from salt-contained hazardous wastewater, is significant to both environment and energy concerns but still challenging due to the high energy cost, severe corrosion, and the absence of competent electrocatalysts. Herein, a novel strategy is proposed for energy-efficient hydrogen production coupled with electro-oxidation removal of ethanolamine pollutant in saline water. To achieve this, an active and durable heterostructured electrocatalyst is developed by in situ growing Ni@Ni S core@shell nanoparticles in cross-linked 3D carbon nanotubes' (CNTs) network, achieving high dispersibility and metallic property, low packing density, and enriched exposed active sites to facilitate fast electron/mass diffusion. The unique Ni@Ni S /CNTs nano-heterostructures are competent for long-term stably electro-oxidizing environmental-unfriendly ethanolamine at a high current density of 100 mA cm in saline water, which not only suppresses oxygen and chloride evolution reactions but also decreases the energy consumption to boost hydrogen production. Associated with experimental results, density functional theory studies indicate that the collaborative adsorption of electrolyte ions and ethanolamine molecules can synergistically modulate the adsorption/desorption properties of catalytic active centers on Ni@Ni S /CNTs surface, leading to long-term stabilized electrocatalysis for efficient ethanolamine oxidation removal and less-energy hydrogen simultaneous production in saline water.
能源危机、环境污染和淡水短缺是地球上的关键问题。从盐水中,特别是从含盐有害废水中电解制氢,对环境和能源问题都具有重要意义,但由于能源成本高、严重腐蚀以及缺乏有效的电催化剂,仍然具有挑战性。在此,我们提出了一种新的策略,用于在盐水中高效制氢并同时电氧化去除乙醇胺污染物。为此,通过在交联的三维碳纳米管(CNTs)网络中原位生长Ni@Ni S核壳纳米颗粒,开发了一种活性和耐久性的异质结构电催化剂,实现了高分散性和金属特性、低堆积密度以及丰富的暴露活性位点,以促进快速的电子/质量扩散。独特的Ni@Ni S /CNTs纳米异质结构能够在盐水中以100 mA cm的高电流密度长期稳定地电氧化环境不友好的乙醇胺,这不仅抑制了析氧和析氯反应,还降低了能耗以促进制氢。结合实验结果,密度泛函理论研究表明,电解质离子和乙醇胺分子的协同吸附可以协同调节Ni@Ni S /CNTs表面催化活性中心的吸附/脱附性能,从而实现长期稳定的电催化,以高效去除乙醇胺并在盐水中同时生产低能耗氢气。