Aug 2026· Chemical Science· 0 citations· 1 references
Medicine
Abstract
The electrochemical nitrate reduction reaction (NO3RR) offers a sustainable route to convert waste NO3− into valuable ammonia (NH3) using renewable electricity. However, the multielectron nature of the NO3RR necessitates the use of efficient, earth-abundant catalysts. While noble metals show high activity, their scarcity motivates the exploration of carbon-based alternatives. Here, we synthesized a triamine derivative based on the triazatrinaphthylene unit (TNP-NH2), a nitrogen-doped planar carbon structure, for the synthesis of six highly porous, crystalline covalent organic frameworks (COFs) as metal-free NO3RR catalysts. All the COFs exhibited good to moderate ammonia yields, achieving the highest yield rate of 2282 µg h−1 mgcat−1 and the highest faradaic efficiency of 82% at −1.0 V vs. RHE. Long-term chronoamperometry confirmed the structural durability of the COF during catalysis. DFT calculations further identified the specific active sites and reaction energetics on the COF backbone responsible for stabilizing key intermediates, consistent with the observed catalytic performance.
Most electrocatalysts reported for the hydrogen evolution reaction (HER) are based on transition-metal composites, nanoparticles, metal-organic frameworks, alloys, sulfides, and metal-nitrogen-carbon frameworks. These materials often require harsh synthetic conditions and generally perform optimally in acidic or alkali...
Prasanna R. Said, A. A. Kumbhar· Journal of Visualized Experi...· 0 citations
The electrocatalytic nitrate reduction reaction (NO3RR) offers significant promise for environmental protection and the production of valuable ammonia (NH3). However, the complexity of the NO3RR process, involving various intermediates and active hydrogen species (Hads), poses challenges to enhancing the selectivity...
Hong Huang, Li-Juan Yu, Song Wan et al.· ACS Sustainable Chemistry &a...· 0 citations
High efficiency and durable non-noble-metal electrocatalysts for the hydrogen evolution reaction (HER) are essential for large-scale green hydrogen production. In this work, a trimetallic polyoxometalate (POM) precursor H2[Co(NH3)6]2[CeMo12O42] (Co2CeMo12) was synthesized via the self-assembly of POM. Subsequently,...
Pingfan Wu, Xiao Feng, Sizhan Shu et al.· Polyoxometalates· 0 citations
The nitrate-to-ammonia electrochemical reduction reaction (NO3RR) driven by renewable energy provides a sustainable route for simultaneous wastewater treatment and green ammonia synthesis. Nevertheless, the NO3RR involves a complex multi-step proton-coupled electron transfer process, and the imbalance between proton su...
Thi Kim Cuong Phu, Thanh Ngoc Pham, Ngan Nguyen Le et al.· RSC Advances· 0 citations
Designing efficient, metal-free covalent organic framework (COF) electrocatalysts is a promising strategy for the oxygen reduction reaction (ORR) due to their structural tunability and stability. Herein, we report two redox-active donor–acceptor COFs, TAPA-DHTD and TTT-DHTD, incorporating a thiophene-based dithiophened...
