Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2019-12-23 , DOI: 10.1016/j.apcatb.2019.118555 Liang Yan , Bing Zhang , Junlu Zhu , Yunyong Li , Panagiotis Tsiakaras , Pei Kang Shen
We report here, an effective strategy to optimize the electronic structure of CoP using copper doping, for greatly enhancing the intrinsic activity and conductivity of CoP in neutral-pH water splitting. As a result, the as-synthesized 3D self-supported Cu-doped CoP nanosheet arrays on carbon paper (Cu-CoP NAs/CP) exhibits admirable electrocatalytic performance toward both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) with overpotentials of 81 and 411 mV at 10 mA cm-2 in 1.0 M PBS (Phosphate Buffer Solution), respectively. Moreover, a neutral electrolyzer, using Cu-CoP NAs/CP as both the anode and cathode, achieves a low cell voltage of 1.72 V at 10 mA cm-2, superior to that of the typical Pt/C||IrO2 couple (1.81 V) and most of the state-of-the-art bifunctional electrocatalysts. Impressively, the electrolyzer can be driven by a single AA battery (∼1.5 V), indicating its practicality in neutral water or seawater splitting. Experimental and density functional theory (DFT) calculations results reveal that the incorporation of Cu into CoP can effectively improve the conductivity and optimize the electronic structure to facilitate the H* adsorption and desorption and the formation of O* intermediates (generated CoOOH active species), thus yielding superior HER and OER catalytic activities. This study opens up a promising way to rationally design highly efficient and low-cost electrocatalysts for electrocatalysis applications.
中文翻译:
通过铜掺杂对磷化钴纳米片阵列进行电子调制,以实现高效的中性pH总体水分解
我们在这里报告了一种有效的策略,可通过掺杂铜来优化CoP的电子结构,以大大提高CoP在中性pH水分解中的固有活性和电导率。结果,在碳纸上合成的3D自支撑Cu掺杂的CoP纳米片阵列(Cu-CoP NAs / CP)对氢气析出反应(HER)和氧气析出反应(OER)均表现出令人赞叹的电催化性能。在1.0 M PBS (磷酸盐缓冲溶液)中在10 mA cm -2时的过电势分别为81和411 mV 。此外,使用Cu-CoP NAs / CP作为阳极和阴极的中性电解槽在10 mA cm -2时可实现1.72 V的低电池电压,优于典型的Pt / C || IrO 2。电偶(1.81 V)和大多数最新的双功能电催化剂。令人印象深刻的是,该电解槽可由单个AA电池(约1.5 V)驱动,这表明该电解槽可用于中性水或海水的分解。实验和密度泛函理论(DFT)的计算结果表明,将Cu掺入CoP可有效提高电导率并优化电子结构,以促进H *的吸附和解吸以及O *中间体(生成的CoOOH活性物质)的形成,因此产生优异的HER和OER催化活性。这项研究为合理设计用于电催化应用的高效,低成本电催化剂开辟了一种有前途的途径。