Efficient and sustainable synthesis of performant metal/nitrogen-doped carbon (M–N–C) catalysts for oxygen reduction and evolution reactions (ORR/OER) is vital for the global switch to green energy technologies–fuel cells and metal–air batteries. This study reports a solid-phase template-assisted mechanosynthesis of Fe–N–C, featuring low-cost and sustainable FeCl3, 2,4,6-tri(2-pyridyl)-1,3,5-triazine (TPTZ), and NaCl. A NaCl-templated Fe-TPTZ metal–organic material was formed using facile liquid-assisted grinding/compression. With NaCl, the Fe-TPTZ template-induced stability allows for a rapid, thus, energy-efficient pyrolysis. Among the produced materials, 3D-FeNC-LAG exhibits remarkable performance in ORR (E 1/2 = 0.85 V and E onset = 1.00 V), OER (E j=10 = 1.73 V), and in the zinc–air battery test (power density of 139 mW cm–2). The multilayer stream mapping (MSM) framework is presented as a tool for creating a sustainability assessment protocol for the catalyst production process. MSM employs time, cost, resource, and energy efficiency as technoeconomic sustainability metrics to assess the potential upstream impact. MSM analysis shows that the 3D-FeNC-LAG synthesis exhibits 90% overall process efficiency and 97.67% cost efficiency. The proposed synthetic protocol requires 2 times less processing time and 3 times less energy without compromising the catalyst efficiency, superior to the most advanced methods.
Bifunctional catalyst materials development for energy storage and conversion technologies is notoriously demanding in terms of electrochemistry (low stability, sluggish kinetics and high total overpotential (∆E)) and logistics (environmental safety, production methodologies and cost). Noble metal electrocatalysts are proven to be good bifunctional catalysts and as a result are being used as benchmark catalysts. However, the environmental and economic sustainability is severely compromised due to the scarcity of these metals. The alternative option is based on first-row transition metal heteroatom-doped carbon materials. Low cost, high availability, great electrocatalytic activity and stability promise to be a suitable noble metal free catalyst for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). This work showcases a high performance Fe-N-C type material with sustainable synthesis and efficient activity towards ORR and OER. Unlike various classical methods for electrocatalyst synthesis, the developed methodology combines mechanochemistry and application of sacrificial template, which yields materials with superior bifunctional oxygen electrocatalytic performance.
Today high-cost Pt-group noble-metal electrocatalysts are still widely applied to effectively overcome the ORR/OER overpotentials.High cost and low abundance alongside poor stability make it necessary to find a replacement for noble-metal-based catalysts to commercialize advanced energy systems successfully. Extensive research of this topic by scientific society resulted in developing various non-noble-metal-based catalysts. Among the recently developed materials, M-N-C catalysts demonstrate great catalytic activity and extraordinary stability, low cost, and a wide variety of sources, making them excellent candidates for replacing Pt-based catalysts.Currently, the most commonly used method for producing M-N-C type catalysts is the carbonization of the precursor material or wet-impregnation of the precursor on carbon support with subsequent carbonization. Additionally, currently available processes often do not meet the current environmental requirements, and the majority of methods are energy-demanding.Here we present a new concept of a facile green method of large-scale synthesis of M-N-C type catalysts with bifunctional electroactivity towards oxygen reduction and evolution reactions.
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