Shang Yunpeng, Feng Kun, Wang Yu, Sun Xuhui, Zhong Jun
Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University Suzhou 215123 China
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences Shanghai 201204 China
RSC Adv. 2019 Apr 12;9(20):11552-11557. doi: 10.1039/c9ra01743g. eCollection 2019 Apr 9.
Ammonia borane (AB) is an ideal hydrogen-storage material for fuel cells but its application has been strongly limited by using rare noble-metal-based catalysts. Here we have prepared a hybrid material of NiCoO nanoparticles on nitric-acid treated carbon nitride (NCN) for the hydrolysis of AB. The NiCoO-NCN catalyst achieves a high total turnover frequency (TOF) value of 76.1 (H) mol per (Cat-metal) mol min in pure water at room temperature, with a good stability by keeping 83.2% activity after 6 runs. The TOF is comparable to the best values ever reported for noble-metal-free catalysts without extra conditions such as light illumination or a strong alkaline environment. Synchrotron radiation based X-ray absorption spectroscopy reveals that the carbon nitride substrate has two reaction centers to form stable interfacial interaction with the NPs, in which carbon can act as the electron acceptor while nitrogen acts as the electron donor. Thus the NP-NCN system has a hybridized electronic structure which is favorable for the catalytic reaction to produce hydrogen. In-depth understanding of the interfacial interaction between NCN and NPs may also shed light on the mechanism study of various energy-related applications based on carbon nitride.
氨硼烷(AB)是一种理想的用于燃料电池的储氢材料,但其应用因使用稀有贵金属基催化剂而受到极大限制。在此,我们制备了一种在硝酸处理的氮化碳(NCN)上负载NiCoO纳米颗粒的杂化材料,用于AB的水解反应。NiCoO-NCN催化剂在室温下的纯水中实现了76.1(H)mol每(Cat-金属)mol每分钟的高总周转频率(TOF)值,并且具有良好的稳定性,经过6次循环后仍保持83.2%的活性。该TOF与无额外条件(如光照或强碱性环境)的无贵金属催化剂所报道的最佳值相当。基于同步辐射的X射线吸收光谱表明,氮化碳基底有两个反应中心与纳米颗粒形成稳定的界面相互作用,其中碳可作为电子受体,而氮作为电子供体。因此,NP-NCN体系具有有利于催化反应产氢的杂化电子结构。深入了解NCN与纳米颗粒之间的界面相互作用,也可能为基于氮化碳的各种能量相关应用的机理研究提供线索。