Double functionalization of N-doped carbon carved hollow nanocubes with mixed metal phosphides as efficient bifunctional catalysts for electrochemical overall water splitting
Double functionalization of N-doped carbon carved hollow nanocubes with mixed metal phosphides as efficient bifunctional catalysts for electrochemical overall water splitting
复制标题
N掺杂碳雕刻中空纳米立方体与混合金属磷化物的双功能化作为电化学整体水分解的高效双功能催化剂
DOI：
10.1016/j.nanoen.2019.103995
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发表时间：
2019-11-01
期刊：
影响因子：
17.6
通讯作者：
Lu, Shih-Yuan
中科院分区：
文献类型：
--
作者：
Lv, Chao-Nan;Zhang, Lei;Lu, Shih-Yuan
开发了一种双功能化方法以产生用于电化学整体水裂解的高效双功能电催化剂。以均匀的Ni-3[Co（CN）（6）]（2）中心点12 H（2）O纳米立方体为原料，通过氨刻、保形聚多巴胺包覆、前驱体金属离子配位、热磷化等工艺制备了双功能催化剂。N掺杂碳雕刻的中空纳米立方体在内部氰化物衍生的碳层中负载有析氢反应（HER）活性（Ni-Co）磷化物，并且在外部聚多巴衍生的碳层上负载有析氧反应（OER）活性（Ni-Fe）磷化物。产物催化剂表现出优异的电解性能，对于OER和HER分别实现251和142 mV的过电位，并且对于全部在10 mA/cm（2）下的总水裂解实现1.63 V的工作电池电压。位于中空立方体的八个顶点处的几十纳米大小的孔允许电解质容易地进入立方体内部并快速排斥从立方体内部产生的气泡。N掺杂的碳纳米立方体提供了快速的电荷传输途径，以及混合金属磷化物产生的正协同效应，显著增强了产物催化剂的催化性能。活性位点的数量和质量都大大提高了双官能化的N掺杂的碳雕刻的中空纳米立方体，这是一个上级催化剂设计的所有电催化应用。
A double functionalization approach was developed to create efficient bifunctional electrocatalysts for electrochemical overall water splitting. Uniform Ni-3[Co(CN)(6)](2)center dot 12H(2)O nanocubes were taken as the starting material to fabricate the bifunctional catalysts through ammonia carving, conformal polydopamine coating, precursor metal ion coordination, and thermal phosphorization. N-doped carbon carved hollow nanocubes were loaded with hydrogen evolution reaction (HER) active (Ni-Co) phosphides in the interior cyanide-derived carbon layers and oxygen evolution reaction (OER) active (Ni-Fe) phosphides on the exterior polydopaimne-derived carbon layers. The product catalyst exhibited excellent electrolytic performances, achieving overpotentials of 251 and 142 mV for the OER and HER, respectively and a working cell voltage of 1.63 V for the overall water splitting all at 10 mA/cm(2). Holes of several tens nanometers in size located at the eight vertices of the hollow cube allow easy access of the electrolyte to and fast rejection of evolving gas bubbles from the interior of the cube. The N-doped carbon nanocubes, providing fast charge transport pathway, and the positive synergistic effects arising from the mixed metal phosphides, significantly enhanced catalytic performances of the product catalyst. Both quantity and quality of the active sites are largely improved with the doubly functionalized N-doped carbon carved hollow nanocubes, which is a superior catalyst design for all electrocatalytic applications.