TY - JOUR
T1 - Carbon-Phosphorus-Nitrogen Materials as Highly Thermally Stable Catalyst Supports for CO2 Hydrogenation to Methanol
AU - Azoulay, Adi
AU - Garcia Baldovi, Alberto
AU - Albero, Josep
AU - Azaria, Noa
AU - Tzadikov, Jonathan
AU - Tashakory, Ayelet
AU - Karjule, Neeta
AU - Hayun, Shmuel
AU - García, Hermenegildo
AU - Shalom, Menny
N1 - Funding Information: This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Programme (grant agreement no. [849068]). The research was partly funded by the following: the Planning & Budgeting Committee/Israel Council for Higher Education (CHE) and Fuel Choice Initiative (Prime Minister Office of Israel), within the framework of “Israel National Research Center for Electrochemical Propulsion” (INREP); the Minerva Center no. 117873; the Israel Science Foundation grant no. 601/21; and the Spanish Ministerio de Economía y Competitividad (MAT2016-77608-C3-1-P and MAT2016-75883-C2-2- P); J.A. and H.G. also gratefully acknowledges financial support from the Spanish Ministry of Economy and Competitiveness (Severo Ochoa SEV2016-0683 and RTI2018-89023-CO2-R1) and by the Generalitat Valenciana (Prometeo 2017-083). Publisher Copyright: © 2022 American Chemical Society.
PY - 2023/1/9
Y1 - 2023/1/9
N2 - The direct conversion of CO2 into methanol through hydrogenation reactions by heterogeneous catalysts is considered a promising green approach for fuel production. The most researched catalyst for methanol formation is Cu, usually in combination with other metals dispersed on different substrates. However, several challenges, such as the low stability, activity, and selectivity of the catalyst, hinder further progress. Here, we present catalysts consisting of Cu and Fe nanoparticles deposited on lightweight carbon-phosphorous-nitrogen (CPN) materials as the support for CO2 hydrogenation to methanol. Detailed analysis reveals a correlation between the elemental composition of the CPN supports and their CO2 adsorption capability, which benefits CO2 conversion to methanol. The unique elemental composition ensures uniform dispersion of both Cu and Fe nanoparticles on CPN and prevents the oxidation of the Cu active sites during the reaction. The best performing sample of the catalysts exhibits a remarkable methanol production yield of 9.82 mol kgcat-1 h-1 at 250 °C under 20 bar, with good methanol selectivity, negligible CO formation, and good stability for 12 h under harsh conditions.
AB - The direct conversion of CO2 into methanol through hydrogenation reactions by heterogeneous catalysts is considered a promising green approach for fuel production. The most researched catalyst for methanol formation is Cu, usually in combination with other metals dispersed on different substrates. However, several challenges, such as the low stability, activity, and selectivity of the catalyst, hinder further progress. Here, we present catalysts consisting of Cu and Fe nanoparticles deposited on lightweight carbon-phosphorous-nitrogen (CPN) materials as the support for CO2 hydrogenation to methanol. Detailed analysis reveals a correlation between the elemental composition of the CPN supports and their CO2 adsorption capability, which benefits CO2 conversion to methanol. The unique elemental composition ensures uniform dispersion of both Cu and Fe nanoparticles on CPN and prevents the oxidation of the Cu active sites during the reaction. The best performing sample of the catalysts exhibits a remarkable methanol production yield of 9.82 mol kgcat-1 h-1 at 250 °C under 20 bar, with good methanol selectivity, negligible CO formation, and good stability for 12 h under harsh conditions.
KW - CO hydrogenation to methanol
KW - Cu−Fe catalyst
KW - heterogeneous catalysis
KW - metal-free material design
KW - supramolecular assembly
KW - thermally stable catalyst support
UR - http://www.scopus.com/inward/record.url?scp=85145607463&partnerID=8YFLogxK
U2 - https://doi.org/10.1021/acsaem.2c03410
DO - https://doi.org/10.1021/acsaem.2c03410
M3 - Article
SN - 2574-0962
VL - 6
SP - 439
EP - 446
JO - ACS Applied Energy Materials
JF - ACS Applied Energy Materials
IS - 1
ER -