Boosting water oxidation on metal-free carbon nanotubes via directional interfacial charge-transfer induced by an adsorbed polyelectrolyte†,Energy & Environmental Science

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Boosting water oxidation on metal-free carbon nanotubes via directional interfacial charge-transfer induced by an adsorbed polyelectrolyte†
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2018-07-02 00:00:00 , DOI: 10.1039/c8ee01487f
Chunshao Mo _{1,

2,

3,

4,

5} , Junhua Jian _{1,

2,

3,

4,

5} , Jing Li _{1,

2,

3,

4,

5} , Zhengsong Fang _{1,

2,

3,

4,

5} , Zhe Zhao _{1,

2,

3,

4,

5} , Zhongke Yuan _{1,

2,

3,

4,

5} , Meijia Yang _{1,

2,

3,

4,

5} , You Zhang _{1,

2,

3,

4,

5} , Liming Dai _{6,

7,

8,

9} , Dingshan Yu _{1,

2,

3,

4,

5}

Affiliation

Engineering the surface and electronic structures of nanocarbons is a viable strategy to boost their catalytic performance. Herein, rather than conventional covalent doping, we used the concept of interfacial charge transfer doping of carbon nanotubes (CNTs) to noncovalently adsorb certain polyelectrolytes (i.e. poly(diallyldimethylammonium chloride), PDDA, acceptor) onto pure CNTs (donor) to act as a buffer layer for richening reactants (OH⁻) via electrostatic interaction and to induce notable interfacial charge redistribution via directional intermolecular charge-transfer, which not only improves the reaction kinetics but also creates a high density of catalytic carbon sites, eventually transforming the inactive CNTs into efficient metal-free water oxidation catalysts. As expected, the resulting PDDA-adsorbed CNT catalysts yielded a remarkably lower overpotential of 370 mV at 10.0 mA cm⁻² with a smaller Tafel slope of 76 mV dec⁻¹ with respect to pure CNTs (>520 mV, 166 mV dec⁻¹), even on a par with the benchmark RuO₂ (360 mV, 137 mV dec⁻¹) in 0.1 M KOH.

中文翻译：

上不含金属的碳纳米管升压水氧化通过由吸附的聚合电解质引起的方向的界面的电荷转移†

对纳米碳的表面和电子结构进行工程设计是提高其催化性能的可行策略。在这里，我们不是使用常规的共价掺杂，而是使用碳纳米管（CNT）的界面电荷转移掺杂的概念，将某些聚电解质（即聚二烯丙基二甲基氯化铵，PDDA，受体）非共价吸附到纯CNT（供体）上，从而充当为反应物富民（OH缓冲层^-）经由静电相互作用并诱导显着的界面电荷再分配经由定向分子间电荷转移，不仅改善了反应动力学，而且还形成了高密度的催化碳位，最终将无活性的CNT转变为有效的无金属水氧化催化剂。如所预期的，所得到的PDDA吸附CNT催化剂产生了在10.0毫安厘米显着降低过电压370毫伏^-2 76毫伏分解的较小塔菲尔斜率^-1相对于纯碳纳米管（> 520毫伏，166毫伏癸^-1），甚至与在0.1 M KOH中的基准RuO ₂（360 mV，137 mV dec ^-1）相当。

更新日期：2018-07-02

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