Environmental Catalysis from First Principles

2010 Spring Symposium

 
Dr. William F. Schnei­der
Pro­fes­sor, Depart­ment of Chem­i­cal and Bio­mol­e­c­u­lar Engi­neer­ing
Con­cur­rent Pro­fes­sor, Depart­ment of Chem­istry and Bio­chem­istry
Uni­ver­si­ty of Notre Dame


Abstract — Het­ero­ge­neous catal­y­sis enabled a rev­o­lu­tion in the 20th cen­tu­ry in terms of mankind’s abil­i­ty to turn moth­er nature’s mate­ri­als into use­ful prod­ucts for soci­ety. In most cas­es, these appli­ca­tions have pre­ced­ed rather than fol­lowed detailed under­stand­ing of cat­alyt­ic mate­ri­als and mech­a­nisms. In order to meet the increas­ing demands of ener­gy sus­tain­abil­i­ty and envi­ron­men­tal pro­tec­tion, catal­y­sis sci­ence and appli­ca­tion in the 21st cen­tu­ry has to be dri­ven by basic insights into how mate­ri­als func­tion and how they can be improved. The advent of first-prin­ci­ples sim­u­la­tions based on den­si­ty func­tion­al the­o­ry (DFT), which are able to reli­ably sim­u­late chem­i­cal struc­tures and reac­tions at the mol­e­c­u­lar scale, has been instru­men­tal in the recent renais­sance in het­ero­ge­neous catal­y­sis research. In this talk, I will illus­trate the capa­bil­i­ties and chal­lenges of apply­ing these sim­u­la­tion tools in the con­text of the cat­alyt­ic chem­istry of nitro­gen oxides (NOx). NOx is an unwant­ed by-prod­uct of com­bus­tion and is par­tic­u­lar­ly dif­fi­cult to remove from lean com­bus­tion sources, such as diesel engines. NOx also has rather com­plex chem­istry that presents spe­cial chal­lenges to sim­u­la­tion. I will describe some of our suc­cess­es in under­stand­ing NOx chem­istry from first-prin­ci­ples, with a par­tic­u­lar empha­sis on recent work to cap­ture the essen­tial fea­tures of the beguil­ing sim­ple cat­alyt­ic oxi­da­tion of NO to NO2 in mol­e­c­u­lar mod­els, to rec­on­cile these mod­els with exper­i­men­tal results, and to use these insights to guide the selec­tion of new and improved cat­a­lysts.

Speaker’s Biog­ra­phy — Bill Schneider’s exper­tise is in chem­i­cal appli­ca­tions of den­si­ty func­tion­al the­o­ry (DFT) sim­u­la­tions. He began his pro­fes­sion­al career in the Ford Motor Com­pa­ny Research Lab­o­ra­to­ry work­ing on a vari­ety of prob­lems relat­ed to the envi­ron­men­tal impacts of auto­mo­bile emis­sions. There he devel­oped an inter­est in the cat­alyt­ic chem­istry of NOx for diesel emis­sions con­trol, and he has pub­lished exten­sive­ly on the chem­istry and mech­a­nisms of NOx decom­po­si­tion, selec­tive cat­alyt­ic reduc­tion, trap­ping, and oxi­da­tion catal­y­sis. In 2004 he joined the Chem­i­cal and Bio­mol­e­c­u­lar Engi­neer­ing fac­ul­ty at the Uni­ver­si­ty of Notre Dame as a tenured Asso­ciate Pro­fes­sor. At Notre Dame he has con­tin­ued his research into the the­o­ry and mol­e­c­u­lar sim­u­la­tion of het­ero­ge­neous catal­y­sis, with par­tic­u­lar empha­sis on reac­tion envi­ron­ment effects on cat­alyt­ic mate­ri­als and their impli­ca­tions for mech­a­nism and reac­tiv­i­ty. He has co-authored more than 90 papers and book chap­ters.