%0 Journal Article
%A Lu, Xiaofei
%A Liu, Yang
%A He, Yurong
%A Kuhn, Andrew N.
%A Shih, Pei-Chieh
%A Sun, Cheng-Jun
%A Wen, Xiaodong
%A Shi, Chuan
%A Yang, Hong
%D 2019
%T Cobalt-Based Nonprecious Metal
Catalysts Derived from
Metal–Organic Frameworks for High-Rate Hydrogenation of Carbon
Dioxide
%U https://acs.figshare.com/articles/journal_contribution/Cobalt-Based_Nonprecious_Metal_Catalysts_Derived_from_Metal_Organic_Frameworks_for_High-Rate_Hydrogenation_of_Carbon_Dioxide/9105119
%R 10.1021/acsami.9b05645.s001
%2 https://acs.figshare.com/ndownloader/files/16605260
%K water gas shift reaction
%K COOH
%K CO 2
%K catalyst
%K Cobalt-Based Nonprecious Metal Catalysts Derived
%K CO 2 conversion rate
%K CO 2 conversion technology
%X The
development of cost-effective catalysts with both high activity
and selectivity for carbon–oxygen bond activation is a major
challenge and has important ramifications for making value-added chemicals
from carbon dioxide (CO2). Herein, we present a one-step
pyrolysis of metal organic frameworks that yields highly dispersed
cobalt nanoparticles embedded in a carbon matrix which shows exceptional
catalytic activity in the reverse water gas shift reaction. Incorporation
of nitrogen into the carbon-based supports resulted in increased reaction
activity and selectivity toward carbon monoxide (CO), likely because
of the formation of a Mott–Schottky interface. At 300 °C
and a high space velocity of 300 000 mL g–1 h–1, the catalyst exhibited a CO2 conversion
rate of 122 μmolCO2 g–1 s–1, eight times higher than that of a reference
Cu/ZnO/Al2O3 catalyst. Our experimental and
computational results suggest that nitrogen-doping lowers the energy
barrier for the formation of formate intermediates (CO2* + H* →
COOH* + *), in addition to the redox mechanism (CO2* + * → CO* + O*). This
enhancement is attributed to the efficient electron transfer at the
cobalt–support interface, leading to higher hydrogenation activity
and opening new avenues for the development of CO2 conversion
technology.
%I ACS Publications