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由豆干衍生的氮和硫掺杂高比表面积碳,作为用于氧还原的可扩展且高效的电催化剂。

N- and S-doped high surface area carbon derived from soya chunks as scalable and efficient electrocatalysts for oxygen reduction.

作者信息

Rana Moumita, Arora Gunjan, Gautam Ujjal K

机构信息

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore 560064, India.

Department of Chemistry, Hansraj College, University of Delhi, Delhi 110007, India.

出版信息

Sci Technol Adv Mater. 2015 Feb 18;16(1):014803. doi: 10.1088/1468-6996/16/1/014803. eCollection 2015 Feb.

Abstract

Highly stable, cost-effective electrocatalysts facilitating oxygen reduction are crucial for the commercialization of membrane-based fuel cell and battery technologies. Herein, we demonstrate that protein-rich soya chunks with a high content of N, S and P atoms are an excellent precursor for heteroatom-doped highly graphitized carbon materials. The materials are nanoporous, with a surface area exceeding 1000 m g, and they are tunable in doping quantities. These materials exhibit highly efficient catalytic performance toward oxygen reduction reaction (ORR) with an onset potential of -0.045 V and a half-wave potential of -0.211 V (versus a saturated calomel electrode) in a basic medium, which is comparable to commercial Pt catalysts and is better than other recently developed metal-free carbon-based catalysts. These exhibit complete methanol tolerance and a performance degradation of merely ∼5% as compared to ∼14% for a commercial Pt/C catalyst after continuous use for 3000 s at the highest reduction current. We found that the fraction of graphitic N increases at a higher graphitization temperature, leading to the near complete reduction of oxygen. It is believed that due to the easy availability of the precursor and the possibility of genetic engineering to homogeneously control the heteroatom distribution, the synthetic strategy is easily scalable, with further improvement in performance.

摘要

高度稳定、具有成本效益的促进氧还原的电催化剂对于基于膜的燃料电池和电池技术的商业化至关重要。在此,我们证明富含蛋白质的大豆块,其含有高含量的N、S和P原子,是杂原子掺杂的高度石墨化碳材料的优异前驱体。这些材料是纳米多孔的,表面积超过1000 m²/g,并且它们的掺杂量是可调节的。这些材料在碱性介质中对氧还原反应(ORR)表现出高效的催化性能,起始电位为-0.045 V,半波电位为-0.211 V(相对于饱和甘汞电极),这与商业Pt催化剂相当,并且优于其他最近开发的无金属碳基催化剂。这些材料表现出完全的甲醇耐受性,并且在最高还原电流下连续使用3000 s后,性能仅下降约5%,而商业Pt/C催化剂下降约14%。我们发现,在较高的石墨化温度下,石墨态N的比例增加,导致氧几乎完全还原。据信,由于前驱体易于获得以及通过基因工程均匀控制杂原子分布的可能性,该合成策略易于扩展,性能还有进一步提升空间。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f292/5036483/e2396729e800/TSTA1166124101.jpg

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