Arc plasma-deposited Co single-atom catalysts supported on an aligned carbon nanofiber for hydrogen peroxide electrosynthesis and an electro-Fenton process

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-07-05 DOI:10.1002/cey2.582
Chang-Kyu Hwang, Sooyeon Kim, Ki Ro Yoon, Thao Thi Le, Chinh V. Hoang, Jae Won Choi, Wenjun Zhang, Sae Yane Paek, Chung Hyeon Lee, Ji Hyun Lee, Keun Hwa Chae, Sohee Jeong, Seung Yong Lee, Byeong-Kwon Ju, Sang Hoon Kim, Sang Soo Han, Jong Min Kim
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Abstract

Atomically dispersed single-atom catalysts (SACs) on carbon supports show great promise for H2O2 electrosynthesis, but conventional wet chemistry methods using particulate carbon blacks in powder form have limited their potential as two-electron (2e) oxygen reduction reaction (ORR) catalysts. Here, we demonstrate high-performance Co SACs supported on a free-standing aligned carbon nanofiber (CNF) using electrospinning and arc plasma deposition (APD). Based on the surface oxidation treatment of aligned CNF and precise control of the deposition amount in a dry-based APD process, we successfully form densely populated Co SACs on aligned CNF. Through experimental analyses and density functional theory calculations, we reveal that Co SAC has a Co–N2–O2 moiety with one epoxy group, leading to excellent 2e ORR activity. Furthermore, the aligned CNF significantly improves mass transfer in flow cells compared to randomly oriented CNF, showing an overpotential reduction of 30 mV and a 1.3-fold improvement (84.5%) in Faradaic efficiency, and finally achieves an outstanding production rate of 15.75 mol gcat−1 h−1 at 300 mA cm−2. The high-performance Co SAC supported on well-aligned CNF is also applied in an electro-Fenton process, demonstrating rapid removal of methylene blue and bisphenol F due to its exceptional 2e ORR activity.

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弧等离子体沉积钴单原子催化剂在排列整齐的碳纳米纤维上的支持,用于过氧化氢电合成和电-芬顿工艺
碳载体上的原子分散单原子催化剂(SACs)在 H2O2 电合成中大有可为,但使用粉末状微粒碳黑的传统湿化学方法限制了它们作为双电子(2e-)氧还原反应(ORR)催化剂的潜力。在这里,我们利用电纺丝和电弧等离子体沉积(APD)技术,展示了支撑在独立排列的碳纳米纤维(CNF)上的高性能 Co SACs。通过对排列整齐的 CNF 进行表面氧化处理,并在干式 APD 过程中精确控制沉积量,我们成功地在排列整齐的 CNF 上形成了高密度的 Co SACs。通过实验分析和密度泛函理论计算,我们发现 Co SAC 具有一个带有环氧基团的 Co-N2-O2 分子,因而具有出色的 2e- ORR 活性。此外,与随机取向的 CNF 相比,对齐的 CNF 显著改善了流动池中的传质,过电位降低了 30 mV,法拉第效率提高了 1.3 倍(84.5%),最终在 300 mA cm-2 的条件下实现了 15.75 mol gcat-1 h-1 的出色生产率。由于其出色的 2e- ORR 活性,支撑在排列整齐的 CNF 上的高性能 Co SAC 还被应用于电-芬顿过程中,显示出其可快速去除亚甲基蓝和双酚 F。
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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
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