TY - JOUR
T1 - Template-Assisted Mechanosynthesis Leading to Benchmark Energy Efficiency and Sustainability in the Production of Bifunctional Fe-N-C Electrocatalysts
AU - Kosimov, Akmal
AU - Alimbekova, Amina
AU - Assafrei, Jurgen Martin
AU - Yusibova, Gulnara
AU - Aruväli, Jaan
AU - Käärik, Maike
AU - Leis, Jaan
AU - Paiste, Päärn
AU - Ahmadi, Majid
AU - Roohi, Khatereh
AU - Taheri, Peyman
AU - Pinto, Sara M.
AU - Cepitis, Ritums
AU - Baptista, Antonio J.
AU - Teppor, Patrick
AU - Lust, Enn
AU - Kongi, Nadezda
N1 - Funding Information:
The present work was financially supported by the Estonian Research Council (grant nos PSG250 and PRG1509). This research was also supported by the EU through the European Regional Development Fund (TK141, “Advanced materials and high-technology devices for energy recuperation systems”).
Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/7/24
Y1 - 2023/7/24
N2 - 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 (E1/2 = 0.85 V and Eonset = 1.00 V), OER (Ej=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.
AB - 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 (E1/2 = 0.85 V and Eonset = 1.00 V), OER (Ej=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.
KW - M−N−C catalyst
KW - oxygen electrocatalysis
KW - sustainable synthesis
KW - template-assisted mechanosynthesis
KW - zinc−air battery
UR - http://www.scopus.com/inward/record.url?scp=85165935929&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.3c02077
DO - 10.1021/acssuschemeng.3c02077
M3 - Article
AN - SCOPUS:85165935929
SN - 2168-0485
VL - 11
SP - 10825
EP - 10834
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
IS - 29
ER -