Research Interest 3:
Design of high-performance catalysts using an integrated theoretical and experimental method
Based on the development of catalysis theory across various materials, we designed a number of promising heterogeneous catalysts using catalytic modeling based upon ab initio calculations and ML. Meanwhile, experimental collaboration plays an essential role in verifying our predictions and providing further insights to help refine our theory. Following a “theoretical design - experimental verification - theoretical generalization” strategy, we successfully designed high-performing catalysts for many industrially significant reactions including i) electrocatalytic reactions (oxygen reduction and evolution, hydrogen evolution, CO2 and nitrogen reduction), ii) thermal liquid-phase reactions (nitrite and nitrate reduction), and iii) vapor-phase reactions (epoxidation, alkene hydrogenation, alcohol decomposition and oxidation).
A notable example is the design of nitrite reduction catalysts for water treatment. There was a huge challenge in the design of nitrite reduction catalyst due to the highly complicated reaction network of this reaction, the variety of product selectivity, and the unknown reaction mechanism. Using catalytic modeling based upon DFT calculations, we for the first time developed the volcano activity models for nitrite reduction, and disentangled the mechanisms of the reaction selectivities. With these new catalysis theories, we successfully designed two sets of promising nitrite reduction catalysts, respectively for the product selectivity toward N2 and NH3. These designed catalysts were then successfully synthesized and tested by experiments which quantitatively verified our predictions. Excitingly, we for the first time discovered a catalyst that achieves near 100% selectivity for nitrite reduction to NH3. More details of these works can be found in Refs. 1-2. This research was recently recognized as the 2020 Best Fundamental Paper by American Institute of Chemical Engineers (AIChE). Most importantly, our works show the predictive power of theory which can be precisely applied to the design of effective energy and environmental catalysts.
Representative Publications:
(1) H. Li, S. Guo, K. Shin, M. S. Wong, and G. Henkelman."Design of a Pd-Au Nitrite Reduction Catalyst by Identifying and Optimizing Active Ensembles", ACS Catalysis, 2019, 9, 7957 (2020 AIChE Best Fundamental Paper Award, Link; ESI Hot & Highly Cited Paper).
(2) H. Li, C. Yan, H. Guo, K. Shin, S. M. Humphrey, C. J. Werth, and G. Henkelman. "CuxIr1-x Nanoalloy Catalysts Achieve Near 100% Selectivity for Aqueous Nitrite Reduction to NH3", ACS Catalysis, 2020, 10, 7915.
Design of high-performance catalysts using an integrated theoretical and experimental method
Based on the development of catalysis theory across various materials, we designed a number of promising heterogeneous catalysts using catalytic modeling based upon ab initio calculations and ML. Meanwhile, experimental collaboration plays an essential role in verifying our predictions and providing further insights to help refine our theory. Following a “theoretical design - experimental verification - theoretical generalization” strategy, we successfully designed high-performing catalysts for many industrially significant reactions including i) electrocatalytic reactions (oxygen reduction and evolution, hydrogen evolution, CO2 and nitrogen reduction), ii) thermal liquid-phase reactions (nitrite and nitrate reduction), and iii) vapor-phase reactions (epoxidation, alkene hydrogenation, alcohol decomposition and oxidation).
A notable example is the design of nitrite reduction catalysts for water treatment. There was a huge challenge in the design of nitrite reduction catalyst due to the highly complicated reaction network of this reaction, the variety of product selectivity, and the unknown reaction mechanism. Using catalytic modeling based upon DFT calculations, we for the first time developed the volcano activity models for nitrite reduction, and disentangled the mechanisms of the reaction selectivities. With these new catalysis theories, we successfully designed two sets of promising nitrite reduction catalysts, respectively for the product selectivity toward N2 and NH3. These designed catalysts were then successfully synthesized and tested by experiments which quantitatively verified our predictions. Excitingly, we for the first time discovered a catalyst that achieves near 100% selectivity for nitrite reduction to NH3. More details of these works can be found in Refs. 1-2. This research was recently recognized as the 2020 Best Fundamental Paper by American Institute of Chemical Engineers (AIChE). Most importantly, our works show the predictive power of theory which can be precisely applied to the design of effective energy and environmental catalysts.
Representative Publications:
(1) H. Li, S. Guo, K. Shin, M. S. Wong, and G. Henkelman."Design of a Pd-Au Nitrite Reduction Catalyst by Identifying and Optimizing Active Ensembles", ACS Catalysis, 2019, 9, 7957 (2020 AIChE Best Fundamental Paper Award, Link; ESI Hot & Highly Cited Paper).
(2) H. Li, C. Yan, H. Guo, K. Shin, S. M. Humphrey, C. J. Werth, and G. Henkelman. "CuxIr1-x Nanoalloy Catalysts Achieve Near 100% Selectivity for Aqueous Nitrite Reduction to NH3", ACS Catalysis, 2020, 10, 7915.