Promoted oxygen reduction kinetics on nitrogen-doped hierarchically porous carbon by engineering proton-feeding centers,Energy & Environmental Science

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Promoted oxygen reduction kinetics on nitrogen-doped hierarchically porous carbon by engineering proton-feeding centers
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-07-13 , DOI: 10.1039/d0ee01613f
Guangbo Chen _{1,

2,

3,

4} , Tao Wang _{5,

6,

7,

8,

9} , Pan Liu _{10,

11,

12,

13} , Zhongquan Liao _{4,

14,

15,

16} , Haixia Zhong _{1,

2,

3,

4} , Gang Wang _{1,

2,

3,

4} , Panpan Zhang _{1,

2,

3,

4} , Minghao Yu _{1,

2,

3,

4} , Ehrenfried Zschech _{4,

14,

15,

16} , Mingwei Chen _{9,

17,

18,

19} , Jian Zhang _{13,

20,

21,

22,

23} , Xinliang Feng _{1,

2,

3,

4}

Affiliation

Center for Advancing Electronics Dresden (Cfaed) and Faculty of Chemistry and Food Chemistry
Technische Universität Dresden
01062 Dresden
Germany
SUNCAT Center for Interface Science and Catalysis
Department of Chemical Engineering
Stanford University
Stanford
USA
School of Chemistry and Chemical Engineering
Shanghai Jiao Tong University
200230 Shanghai
P. R. China
Fraunhofer Institute for Ceramic
Technologies and Systems (IKTS)
01109 Dresden
Department of Materials Science and Engineering
Johns Hopkins University
Baltimore
Department of Applied Chemistry
School of Applied and Natural Sciences
Northwestern Polytechnical University
Xi'an

Electrocatalytic oxygen reduction reaction (ORR) is the vital process for next-generation electrochemical energy storage and conversion technologies, e.g., metal–air batteries and fuel cells. During the ORR, the O₂* and O* intermediates principally combine with protons to form OOH* and OH* species, respectively, which are the proton-coupled electron transfer processes. Unfortunately, under alkaline conditions, the protons are essentially generated from the sluggish water dissociation process, which unavoidably limits the ORR kinetics. Herein, we design and synthesize a nitrogen-doped hierarchically porous carbon with homogeneously distributed ultrafine α-MoC nanoparticles (α-MoC/NHPC) as a model electrocatalyst. Theoretical investigations unveil that α-MoC on NHPC could efficiently reduce the energy barrier of the water dissociation process to generate protons, eventually promoting the proton-coupled ORR kinetics. In a 0.1 M KOH aqueous solution, α-MoC/NHPC exhibits excellent ORR performance with a high half-wave potential of 0.88 V (VS. reversible hydrogen electrode), which outperforms those for NHPC and commercial Pt/C. Moreover, as the air electrode in a zinc-air battery, α-MoC/NHPC presents a large peak power density of 200.3 mW cm⁻² and long-term stability. Thereby, our approach to engineering proton-feeding centers paves a new avenue towards the understanding of ORR kinetics and the development of high-performance ORR electrocatalysts.

中文翻译：

通过工程质子进料中心促进掺氮分级多孔碳的氧还原动力学

电催化氧还原反应（ORR）是下一代电化学能量存储和转换技术（例如金属-空气电池和燃料电池）的重要过程。在ORR期间，O ₂*和O *中间体主要与质子结合形成OOH *和OH *物质，这是质子耦合的电子转移过程。不幸的是，在碱性条件下，质子基本上是由缓慢的水离解过程产生的，这不可避免地限制了ORR动力学。本文中，我们设计并合成了均匀分布的超细α-MoC纳米颗粒（α-MoC/ NHPC）作为模型电催化剂的氮掺杂的分级多孔碳。理论研究表明，NHPC上的α-MoC可以有效降低水离解过程产生质子的能垒，最终促进质子偶联的ORR动力学。在0.1 M KOH水溶液中，α-MoC/ NHPC具有极好的ORR性能，且半波电势高达0.88 V（VS。可逆氢电极），其性能优于NHPC和商用Pt / C。此外，作为锌-空气电池中的空气电极，α-MoC/ NHPC具有200.3 mW cm^-2的大峰值功率密度和长期稳定性。因此，我们设计质子进料中心的方法为了解ORR动力学和开发高性能ORR电催化剂开辟了一条新途径。

更新日期：2020-09-16

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