Dataset Information

Interfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols.

ABSTRACT: Long-chain alcohols synthesis (LAS, C5+OH) from syngas provides a promising route for the conversion of coal/biomass/natural gas into high-value chemicals. Cu-Fe binary catalysts, with the merits of cost effectiveness and high CO conversion, have attracted considerable attention. Here we report a nano-construct of a Fe5C2-Cu interfacial catalyst derived from Cu4Fe1Mg4-layered double hydroxide (Cu4Fe1Mg4-LDH) precursor, i.e., Fe5C2 clusters (~2?nm) are immobilized onto the surface of Cu nanoparticles (~25?nm). The interfacial catalyst exhibits a CO conversion of 53.2%, a selectivity of 14.8?mol% and a space time yield of 0.101?g gcat-1 h-1 for long-chain alcohols, with a surprisingly benign reaction pressure of 1?MPa. This catalytic performance, to the best of our knowledge, is comparable to the optimal level of Cu-Fe catalysts operated at much higher pressure (normally above 3?MPa).

SUBMITTER: Li Y

PROVIDER: S-EPMC6941981 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Interfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols.

Li Yinwen Y Gao Wa W Peng Mi M Zhang Junbo J Sun Jialve J Xu Yao Y Hong Song S Liu Xi X Liu Xingwu X Wei Min M Zhang Bingsen B Ma Ding D

Nature communications 20200103 1

Long-chain alcohols synthesis (LAS, C5+OH) from syngas provides a promising route for the conversion of coal/biomass/natural gas into high-value chemicals. Cu-Fe binary catalysts, with the merits of cost effectiveness and high CO conversion, have attracted considerable attention. Here we report a nano-construct of a Fe5C2-Cu interfacial catalyst derived from Cu4Fe1Mg4-layered double hydroxide (Cu4Fe1Mg4< ...[more]

PMID: 31900400

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Project description:The development of efficient catalysts is one of the main challenges in CO2 conversion to valuable chemicals and fuels. Herein, inspired by the knowledge of the thermocatalytic (TC) processes, Cu/ZnO and bare Cu catalysts enriched with Cu+1 were studied to convert CO2 via the electrocatalytic (EC) pathway. Integrating Cu with ZnO (a CO-generation catalyst) is a strategy explored in the EC CO2 reduction to reduce the kinetic barrier and enhance C-C coupling to obtain C2+ chemicals and energy carriers. Herein, ethanol was produced with the Cu/ZnO catalyst, reaching a productivity of about 5.27 mmol·gcat-1·h-1 in a liquid-phase configuration at ambient conditions. In contrast, bare copper preferentially produced C1 products like formate and methanol. During CO2 hydrogenation, a methanol selectivity close to 100% was achieved with the Cu/ZnO catalysts at 200 °C, a value that decreased at higher temperatures (i.e., 23% at 300 °C) because of thermodynamic limitations. The methanol productivity increased to approximately 1.4 mmol·gcat-1·h-1 at 300 °C. Ex situ characterizations after testing confirmed the potential of adding ZnO in Cu-based materials to stabilize the Cu1+/Cu0 interface at the electrocatalyst surface because of Zn and O enrichment by an amorphous zinc oxide matrix; while in the TC process, Cu0 and crystalline ZnO prevailed under CO2 hydrogenation conditions. It is envisioned that the lower *CO binding energy at the Cu0 catalyst surface in the TC process than in the Cu1+ present in the EC one leads to preferential CO and methanol production in the TC system. Instead, our EC results revealed that an optimum local CO production at the ZnO surface in tandem with a high amount of superficial Cu1+ + Cu0 species induces ethanol formation by ensuring an appropriate local amount of *CO intermediates and their further dimerization to generate C2+ products. Optimizing the ZnO loading on Cu is proposed to tune the catalyst surface properties and the formation of more reduced CO2 conversion products.

Dataset Information

Interfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols.

Publications

Interfacial Fe<sub>5</sub>C<sub>2</sub>-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols.

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