{Reference Type}: Journal Article
{Title}: Hydrogen cyanide catalytic hydrolysis mechanism by Al-doped graphene: A density functional theory study.
{Author}: Yang F;Tian S;Ning P;Wang B;Xiang Y;Song X;Yang H;
{Journal}: J Mol Model
{Volume}: 30
{Issue}: 1
{Year}: 2024 Jan 3
{Factor}: 2.172
{DOI}: 10.1007/s00894-023-05822-y
{Abstract}: <B>BACKGROUND: </B>The hydrogen cyanide (HCN) hydrolysis reaction mechanism over Al-doped graphene was investigated through the density functional theory method. HCN preferentially adsorbed vertically on the Al top site to form a stable adsorption configuration. H2O preferentially adsorbed parallel on the Al top site to form a stable adsorption configuration. The competitive adsorption of HCN and H2O weakened the adsorption stability of each molecule over Al-doped graphene. The break of C-N and H-O bonds was the key process in the preferential fracture pathway of the C-H bond. The break of C-N and C-H bonds was the key process in the preferential fracture pathway of the H-O bond. HCN played the role of bridge in the joint adsorption process. H atom transfer and C-N bond cleavage promoted the generation of CO and NH3. The change in the order of H atom transfer determined the reaction energy barrier. NH2CHO was more likely to act as an intermediate to promote the hydrolysis process.<BR><B>METHODS: </B>The calculation work was achieved from the Dmol3 program in Material Studio 2017 using the GGA/PBE method with DNP basis, including the geometric structure and reaction pathway optimization, and adsorption energy calculation. All calculations were performed using a spin-polarized set and the TS method was used for DFT-D correction.