TY - JOUR A1 - Qin, Qing A1 - Oschatz, Martin T1 - Overcoming chemical inertness under ambient conditions BT - a critical view on recent developments in Ammonia synthesis via electrochemical N-2 reduction by asking five questions JF - ChemElectroChem N2 - Ammonia (NH3) synthesis by the electrochemical N-2 reduction reaction (NRR) is increasingly studied and proposed as an alternative process to overcome the disadvantages of Haber-Bosch synthesis by a more energy-efficient, carbon-free, delocalized, and sustainable process. An ever-increasing number of scientists are working on the improvement of the faradaic efficiency (FE) and NH3 production rate by developing novel catalysts, electrolyte concepts, and/or by contributing theoretical studies. The present Minireview provides a critical view on the interplay of different crucial aspects in NRR from the electrolyte, over the mechanism of catalytic activation of N-2, to the full electrochemical cell. Five critical questions are asked, discussed, and answered, each coupled with a summary of recent developments in the respective field. This article is not supposed to be a complete summary of recent research about NRR but provides a rather critical personal view on the field. It is the major aim to give an overview over crucial influences on different length scales to shine light on the sweet spots into which room for revolutionary instead of incremental improvements may exist. KW - N-2 reduction KW - ammonia synthesis KW - catalysis KW - catalysts KW - electrolytes Y1 - 2022 U6 - https://doi.org/10.1002/celc.201901970 SN - 2196-0216 VL - 7 IS - 4 SP - 878 EP - 889 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Qin, Qing A1 - Heil, T. A1 - Schmidt, J. A1 - Schmallegger, Max A1 - Gescheidt, Georg A1 - Antonietti, Markus A1 - Oschatz, Martin T1 - Electrochemical Fixation of Nitrogen and Its Coupling with Biomass Valorization with a Strongly Adsorbing and Defect Optimized Boron-Carbon-Nitrogen Catalyst JF - ACS Applied Energy Materials N2 - 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 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. KW - non-metal catalysis KW - porous carbon KW - heteroatoms KW - N-2 reduction KW - HMF oxidation Y1 - 2019 U6 - https://doi.org/10.1021/acsaem.9b01852 SN - 2574-0962 VL - 2 IS - 11 SP - 8359 EP - 8365 PB - American Chemical Society CY - Washington ER -