Jiang Binbin, Huang Aijian, Wang Tao, Shao Qi, Zhu Wenxiang, Liao Fan, Cheng Yafei, Shao Mingwang
Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, PR China; Anhui Key Laboratory of Photoelectric-Magnetic Functional Materials, School of Chemistry and Chemical Engineering, Anqing Normal University, Anqing 246011, China.
School of Electronics Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, PR China; Department of Chemistry, Tsinghua University, Beijing 100084, China.
J Colloid Interface Sci. 2020 Jul 1;571:30-37. doi: 10.1016/j.jcis.2020.03.022. Epub 2020 Mar 9.
Exploring the highly efficient and durable electrocatalysts for hydrogen evolution reaction (HER) is vitally necessary for sustainable energy conversion and storage system. Herein, we fabricate an interfacial engineered Rh-carbon nitride as advanced electrocatalysts for HER in the acidic and alkaline electrolytes. The interface between Rh nanocrystals and carbon nitride may adjust the electronic structure of Rh, which results in high activity for HER. The optimal Rh-carbon nitride shows low overpotential at current density of -10 mA·cm and small Tafel slope (13 mV and 25.0 mV dec in 0.5 M HSO, 46 mV and 42.0 mV dec in 1.0 M KOH, respectively), which is superior to that of commercial Pt/C (21 mV and 28.5 mV dec in 0.5 M HSO, 55 mV and 44.0 mV dec in 1.0 M KOH, respectively). Importantly, this composite also exhibits long-term stability in 0.5 M HSO and 1.0 M KOH. The excellent HER performances can be attribute to the interface between Rh and carbon nitride, which downshifts their d-band center positions, tuning the adsorption ability for hydrogen and accelerating the HER kinetics. This work may open up an efficient method to design metal/carbon hybrid for electrocatalysis.
探索用于析氢反应(HER)的高效耐用的电催化剂对于可持续能源转换和存储系统至关重要。在此,我们制备了一种界面工程化的Rh-碳氮化物作为在酸性和碱性电解质中用于HER的先进电催化剂。Rh纳米晶体与碳氮化物之间的界面可能会调整Rh的电子结构,从而导致HER具有高活性。最佳的Rh-碳氮化物在电流密度为-10 mA·cm时显示出低过电位以及小的塔菲尔斜率(在0.5 M H₂SO₄中分别为13 mV dec⁻¹和25.0 mV dec⁻¹,在1.0 M KOH中分别为46 mV dec⁻¹和42.0 mV dec⁻¹),这优于商业Pt/C(在0.5 M H₂SO₄中分别为21 mV dec⁻¹和28.5 mV dec⁻¹,在1.0 M KOH中分别为55 mV dec⁻¹和44.0 mV dec⁻¹)。重要的是,这种复合材料在0.5 M H₂SO₄和1.0 M KOH中也表现出长期稳定性。优异的HER性能可归因于Rh与碳氮化物之间的界面,该界面降低了它们的d带中心位置,调节了对氢的吸附能力并加速了HER动力学。这项工作可能会开辟一种设计用于电催化的金属/碳杂化物的有效方法。