Strengthening the Metal Center of Co–N4 Active Sites in a 1D–2D Heterostructure for Nitrate and Nitrogen Reduction Reaction to Ammonia,ACS Sustainable Chemistry & Engineering

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Strengthening the Metal Center of Co–N4 Active Sites in a 1D–2D Heterostructure for Nitrate and Nitrogen Reduction Reaction to Ammonia
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-04-10 , DOI: 10.1021/acssuschemeng.2c07114
Sourav Paul ₁ , Sougata Sarkar ₁ , Ashadul Adalder ₁ , Samadhan Kapse ₂ , Ranjit Thapa ₂ , Uttam Kumar Ghorai ₁

Affiliation

Ammonia forms the fundamental agricultural constituent and vital energy provenance of a clean hydrogen mediator. Ammonia production leads to immense energy utilization and drastic environmental repercussion. It is a daunting task to design and synthesize competent catalysts for reduction of nitrogenous species (nitrogen or nitrates, by the nitrogen reduction reaction (NRR) or nitrate reduction reaction (NO₃RR) process, respectively) into ammonia. Cobalt(II) phthalocyanine (CoPc) nanotubes were effectively wrapped by 2D graphene sheets to produce a (1D–2D) heterostructure catalyst, which plays the role of a competent electrocatalyst for the NRR as well as NO₃RR. The electrocatalyst showed an ammonia yield rate and a Faradaic efficiency of 58.82 μg h^–1 mg^–1_cat and 95.12%, respectively, for the NO₃RR and for NRR 143.38 μg h^–1 mg^–1_cat and 43.69%, respectively. Bader charge investigation revealed the transport of charge to Co–N₄ active sites from reduced graphene oxide (RGO), which aids during the production of intermediates NNH* for nitrogen reduction and *NOH for nitrate reduction along with suppression of the parasitic HER, thereby demonstrating good selectivity and Faradaic efficiency. This work showcases new mechanistic discernment about the role of work function, interfacial charge transport, and electrocatalytic overpotential for the nitrogen/nitrate reduction reaction.

中文翻译：

在 1D-2D 异质结构中强化 Co-N4 活性位点的金属中心，用于硝酸盐和氮还原氨反应

氨是清洁氢介质的基本农业成分和重要能源来源。氨生产导致巨大的能源利用和剧烈的环境影响。设计和合成用于将含氮物质（氮或硝酸盐，分别通过氮还原反应 (NRR) 或硝酸盐还原反应 (NO 3 RR) 过程）还原成氨的有效催化剂是一项艰巨的_任务。钴 (II) 酞菁 (CoPc) 纳米管被 2D 石墨烯片有效包裹以产生 (1D–2D) 异质结构催化剂，该催化剂对 NRR 和 NO 3 RR 起着良好电催化剂的_作用。该电催化剂的氨产率和法拉第效率为 58.82 μg h ^–1 mg对于 NO ₃ RR 和 NRR 143.38 μg h ^–1 mg ，分别为^–1_{cat和 95.12%}^–1_cat和 43.69%。Bader 电荷调查揭示了电荷从还原氧化石墨烯 (RGO) 传输到 Co–N 4 活性位点，这有助于生产用于氮还原的中间体 NNH* 和用于硝酸盐还原的 *NOH 以及抑制寄生 HER，_从而表现出良好的选择性和法拉第效率。这项工作展示了关于功函数、界面电荷传输和电催化过电势对氮/硝酸盐还原反应的作用的新的机理认识。

更新日期：2023-04-10

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