Electrochemical Fixation of Nitrogen and Its Coupling with Biomass Valorization with a Strongly Adsorbing and Defect Optimized Boron-Carbon-Nitrogen Catalyst

  • The electrochemical conversion of low-cost precursors into high-value chemicals using renewably generated electricity is a promising approach to build up an environmentally friendly energy cycle, including a storage element. The large-scale implementation of such process can, however, only be realized by the design of cost-effective electrocatalysts with high efficiency and highest stability. Here, we report the synthesis of N and B codoped porous carbons. The constructed B-N motives combine abundant unpaired electrons and frustrated Lewis pairs (FLPs). They result in desirable performance for electrochemical N-2 reduction reaction (NRR) and electrooxidation of 5-hydroxymethylfurfural (HMF) in the absence of any metal cocatalyst. A maximum Faradaic efficiency of 15.2% with a stable NH3 production rate of 21.3 mu g h(-1) mg(-1) is obtained in NRR. Besides, 2,5-furandicarboxylic acid (FDCA) is first obtained by using non-metalbased electrocatalysts at a conversion of 71% and with yield of 57%. Gas adsorption experiments elucidate theThe electrochemical conversion of low-cost precursors into high-value chemicals using renewably generated electricity is a promising approach to build up an environmentally friendly energy cycle, including a storage element. The large-scale implementation of such process can, however, only be realized by the design of cost-effective electrocatalysts with high efficiency and highest stability. Here, we report the synthesis of N and B codoped porous carbons. The constructed B-N motives combine abundant unpaired electrons and frustrated Lewis pairs (FLPs). They result in desirable performance for electrochemical N-2 reduction reaction (NRR) and electrooxidation of 5-hydroxymethylfurfural (HMF) in the absence of any metal cocatalyst. A maximum Faradaic efficiency of 15.2% with a stable NH3 production rate of 21.3 mu g h(-1) mg(-1) is obtained in NRR. Besides, 2,5-furandicarboxylic acid (FDCA) is first obtained by using non-metalbased electrocatalysts at a conversion of 71% and with yield of 57%. Gas adsorption experiments elucidate the relationship between the structure and the ability of the catalysts to activate the substrate molecules. This work opens up deep insights for the rational design of non-metal-based catalysts for potential electrocatalytic applications and the possible enhancement of their activity by the introduction of FLPs and point defects at grain boundaries.show moreshow less

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Metadaten
Author:Qing QinORCiDGND, T. Heil, J. Schmidt, Max SchmalleggerORCiD, Georg GescheidtORCiD, Markus AntoniettiORCiDGND, Martin OschatzORCiDGND
DOI:https://doi.org/10.1021/acsaem.9b01852
ISSN:2574-0962
Parent Title (English):ACS Applied Energy Materials
Publisher:American Chemical Society
Place of publication:Washington
Document Type:Article
Language:English
Year of first Publication:2019
Year of Completion:2019
Release Date:2020/10/11
Tag:HMF oxidation; N-2 reduction; heteroatoms; non-metal catalysis; porous carbon
Volume:2
Issue:11
Pagenumber:13
First Page:8359
Last Page:8365
Funder:Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under 2008/1, 390540038]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften
Peer Review:Referiert
Publication Way:Open Access
Open Access / Hybrid Open-Access