Diethylenetriamine-mediated self-assembly of three-dimensional hierarchical nanoporous CoP nanoflowers/pristine graphene interconnected networks as efficient electrocatalysts toward hydrogen evolution,Sustainable Energy & Fuels

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Diethylenetriamine-mediated self-assembly of three-dimensional hierarchical nanoporous CoP nanoflowers/pristine graphene interconnected networks as efficient electrocatalysts toward hydrogen evolution
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2017-10-09 00:00:00 , DOI: 10.1039/c7se00454k
Xiuling Fan _{1,

2,

3,

4,

5} , Xiaoyan Wang _{1,

2,

3,

4,

5} , Weiyong Yuan _{1,

2,

3,

4,

5} , Chang Ming Li _{1,

2,

3,

4,

5}

Affiliation

Highly active, durable, and low-cost hydrogen evolution reaction (HER) catalysts are critical for large-scale energy storage in the form of hydrogen through water splitting but their fabrication presents great challenges. Herein we report the synthesis of a novel 3D hierarchical nanoporous CoP nanoflowers/pristine graphene interconnected network structure via diethylenetriamine (DETA)-mediated self-assembly, in which DETA promoted the uniform dispersion of graphene and the nucleation of the CoP precursor on graphene, the seed aggregation facilitated the formation of nanoflowers and a 3D network, and the gas release during the low-temperature phosphidation produced nanopores inside the nanoflowers. This nanoarchitecture shows an onset potential of −0.014 V, an overpotential of 98.1 mV to achieve 10 mA cm⁻², a Tafel slope of 40.9 mV dec⁻¹, and an exchange current density of 0.119 mA cm⁻². The onset overpotential, overpotential to achieve 10 mA cm⁻², and Tafel slope are all among the lowest reported for non-noble metal hydrogen evolution reaction (HER) catalysts, and the exchange current density also compares favorably to those of most reported HER catalysts. In addition, the catalyst exhibits excellent durability with negligible loss in current density after 2000 cyclic voltammetry (CV) cycles (+0.01 to −0.17 V vs. the RHE, at a scan rate of 100 mV s⁻¹) or 23.5 h of chronoamperometric measurement at an overpotential of 98.1 mV, and a high faradaic efficiency of close to 100%. This work not only creates a high-performance and inexpensive HER electrocatalyst by utilizing the great advantages of 3D hierarchically nanostructured networks, but also develops a facile and economical strategy for the self-assembly of hierarchical nanostructures and offers scientific insight into its mechanism.

中文翻译：

二亚乙基三胺介导的三维分层纳米多孔CoP纳米花/原始石墨烯互连网络的自组装，作为通向氢释放的有效电催化剂

高活性，耐用且低成本的析氢反应（HER）催化剂对于通过水分解制氢形式的大规模储能至关重要，但其制造面临巨大挑战。本文中，我们报告了通过二亚乙基三胺（DETA）介导的自组装合成新型3D分层纳米多孔CoP纳米花/原始石墨烯互连网络结构，其中DETA促进了石墨烯的均匀分散和CoP前体在石墨烯上的成核，种子聚集促进了纳米花和3D网络的形成，并且在低温磷酸化过程中释放的气体在纳米花内部产生了纳米孔。这种纳米结构显示的起始电势为-0.014 V，过电势为98.1 mV，可实现10 mA cm^-2，Tafel斜率为40.9 mV dec^-1，交换电流密度为0.119 mA cm^-2。起始过电势，达到10 mA cm^-2的过电势和Tafel斜率均在非贵金属氢析出反应（HER）催化剂中报道的最低值中，并且交换电流密度也与大多数报道的HER催化剂相比是有利的。此外，该催化剂在以100 mV s^-1的扫描速率进行2000次循环伏安（CV）循环（相对RHE为+0.01至-0.17 V）后，具有出色的耐久性，且电流密度损失可忽略不计）或23.5 h的计时安培测量，在98.1 mV的超电势下，法拉第效率接近100％。这项工作不仅通过利用3D分层纳米结构网络的巨大优势创建了一种高性能且价格便宜的HER电催化剂，而且还为分层纳米结构的自组装开发了一种简便而经济的策略，并对其机理提供了科学见解。

更新日期：2017-10-26

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