Article, 2024

Uniting Synergistic Effect of Single‐Ni Site and Electric Field of B‐ Bridged‐N for Boosted Electrocatalytic Nitrate Reduction to Ammonia

Small, ISSN 1613-6829, 1613-6810, Page e2310082, 10.1002/smll.202310082

Contributors

Ajmal, Saira 0000-0001-7504-230X [1] Kumar, Anuj 0000-0001-9374-6677 [2] Mushtaq, Muhammad Asim 0000-0002-1941-4719 [1] Tabish, Mohammad 0000-0003-1702-2671 [3] Zhao, Yulin [4] Zhang, Wenbin [1] Khan, Abdul Sammed [1] Saad, Ali 0000-0002-4528-8349 [5] Yasin, Ghulam 0000-0001-8794-3965 (Corresponding author) [1] Zhao, Wei 0000-0001-5407-6164 (Corresponding author) [1]

Affiliations

  1. [1] Shenzhen University
    2. [NORA names: China; Asia, East];
  2. [2] GLA University
    3. [NORA names: India; Asia, South];
  3. [3] Beijing University of Chemical Technology
    4. [NORA names: China; Asia, East];
  4. [4] Southwest University of Science and Technology
    5. [NORA names: China; Asia, East];
  5. [5] Aarhus University
    6. [NORA names: AU Aarhus University; University; Denmark; Europe, EU; Nordic; OECD]

Abstract

Electrochemical conversion of nitrate, a prevalent water pollutant, to ammonia (NH3 ) is a delocalized and green path for NH3 production. Despite the existence of different nitrate reduction pathways, selectively directing the reaction pathway on the road to NH3 is now hindered by the absence of efficient catalysts. Single-atom catalysts (SACs) are extensively investigated in a wide range of catalytic processes. However, their application in electrocatalytic nitrate reduction reaction (NO3 - RR) to NH3 is infrequent, mostly due to their pronounced inclination toward hydrogen evolution reaction (HER). Here, Ni single atoms on the electrochemically active carrier boron, nitrogen doped-graphene (BNG) matrix to modulate the atomic coordination structure through a boron-spanning strategy to enhance the performance of NO3 - RR is designed. Density functional theory (DFT) study proposes that BNG supports with ionic characteristics, offer a surplus electric field effect as compared to N-doped graphene, which can ease the nitrate adsorption. Consistent with the theoretical studies, the as-obtained NiSA@BNG shows higher catalytic activity with a maximal NH3 yield rate of 168 µg h-1  cm-2 along with Faradaic efficiency of 95% and promising electrochemical stability. This study reveals novel ways to rationally fabricate SACs' atomic coordination structure with tunable electronic properties to enhance electrocatalytic performance.

Keywords

BNG, Faradaic efficiency, N-doped graphene, Ni single atoms, absence, activity, adsorption, ammonia, atomic coordination structure, atoms, boron, catalyst, catalytic activity, catalytic process, characteristics, conversion of nitrate, coordination structure, density, density functional theory, doped-graphene, effect, efficiency, efficient catalyst, electric field, electric field effect, electricity, electrocatalytic nitrate reduction, electrocatalytic nitrate reduction reaction, electrocatalytic performance, electrochemical conversion, electrochemical conversion of nitrate, electrochemical stability, electrochemically, electronic properties, evolution reaction, field effects, functional theory, graphene, green path, hydrogen, hydrogen evolution reaction, inclination, ionic characteristics, nitrate, nitrate adsorption, nitrate reduction, nitrate reduction pathway, nitrate reduction reaction, nitrogen, novel ways, path, pathway, performance, pollution, process, production, properties, rate, reaction, reaction pathways, reduction, reduction pathway, reduction reaction, road, single atoms, single-atom catalysts, sites, stability, strategies, structure, study, synergistic effect, theoretical study, theory, water pollution, way, yield rate

Funders

  • National Natural Science Foundation of China

Data Provider: Digital Science

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