期刊
ACS CATALYSIS
卷 9, 期 3, 页码 2633-2638出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b04896
关键词
rational design; heterogeneous catalyst; reaction kinetics; chemical potential; optimal adsorption energy
资金
- NSFC [21333003, 21622305, 201703067, 21873028, 21832002]
- National Key R&D Program of China [2018YFA0208602]
- National Ten Thousand Talent Program for Young Top-notch Talents in China
- Shanghai ShuGuang project [17SG30]
- Postdoctoral Science Foundation of China [2017M611471]
In silico design of catalysts has made significant progress in recent decades. Arguably the best one among the used methods is to plot the activity against the adsorption energy of the key intermediate (E-ad), usually leading to a volcano-shaped trend, on the peak of which the optimal adsorption energy (E-ad(opt)) can be identified for locating the best catalyst. However, E-ad(opt) has not been clearly understood, and its application for catalyst screening mainly relies on massive quantum-chemical calculations. Here, we derive a simple yet efficient method to estimate E-ad(opt) in heterogeneous catalysis based on an elegant kinetic formulism expressed by the notation of chemical potentials and a generalized two-step model. With this method, (i) E-ad(opt) can be estimated without quantum-chemical calculations, and one can even calculate it by hand from gas-phase thermodynamic data; (ii) some important trends for catalyst design and optimal reaction conditions can be readily derived; and (iii) many previous findings in reaction kinetics can be easily integrated in our formulism with clearer physical pictures. This work could pave a simple way for efficient design of heterogeneous catalysts.
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