東華大學圖書館 |

Language: English

Help

回圖書館首頁

手機版館藏查詢

Back

Switch To: Labeled | MARC Mode | ISBD

Grand Canonical Approach to Modeling...

Zhang, Zisheng.

Linked to FindBook

Google Book

Amazon

博客來

Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces./
Author:	Zhang, Zisheng.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2024,
Description:	284 p.
Notes:	Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
Contained By:	Dissertations Abstracts International85-11B.
Subject:	Computational chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31296762
ISBN:	9798382769103

Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces.
Zhang, Zisheng.

Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces. - Ann Arbor : ProQuest Dissertations & Theses, 2024 - 284 p.

Source: Dissertations Abstracts International, Volume: 85-11, Section: B.

Thesis (Ph.D.)--University of California, Los Angeles, 2024.

Dynamic structural rearrangement has been observed in a wide range of heterogeneous catalysts and functional materials when they are in operation. Such fluxional behaviors underlie the reactivity, activation, or deactivation in various catalytic systems. However, experimentally resolving their atomic structures has been challenging due to the transient and minority nature of the metastable motifs and surface phases. The role of theory in investigating those dynamic systems hence remains singular.This dissertation will focus on the development and application of a grand canonical (GC) approach to model catalysts that undergo significant off-stoichiometric restructurings in reaction conditions. Grand canonical genetic algorithm (GCGA), an efficient global optimization algorithm, is implemented and used to explore the vast chemical space of cluster isomerization, surface atoms rearrangement, mixed coverage and configuration of adsorbates, and to locate the global and relevant local minima. The found minima constitute a GC ensemble of catalyst states that are diverse in structure, stoichiometry, and reactivity. By ab initio thermodynamics and grand canonical density functional theory (GC-DFT) calculations, the dependence on reaction conditions (temperature, partial pressures, pH, electrode potential, solute concentrations, etc.) can be included into the free energetics of the states, to probe how the distribution of states responds to varying conditions.This approach has been applied to investigate multiple systems ranging from thermal to electro-catalysis, and from supported clusters to extended surfaces. This talk will cover a few representative systems, including boron nitride in thermal oxidative dehydrogenation conditions, supported sub-nanometer metal clusters in electrocatalysis, and copper electrodes in electroreduction conditions. The dissertation works will illustrate how the GC approach not only helps interpret complex experimental observations, but also provides rich atomic insights into the structure and reactivity of catalytic species, and lays the foundation to build a new paradigm for reaction kinetics, catalyst optimization, non-equilibrium behaviors, and more.

ISBN: 9798382769103Subjects--Topical Terms:

3350019
Computational chemistry.
Subjects--Index Terms:

Catalysis

Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces.
LDR:03460nmm a2200397 4500 001 2403670
005 20241118135909.5
006 m o d
007 cr#unu||||||||
008 251215s2024 ||||||||||||||||| ||eng d
020 $a 9798382769103
035 $a (MiAaPQ)AAI31296762
035 $a AAI31296762
040 $a MiAaPQ $c MiAaPQ
100 1 $a Zhang, Zisheng. $3 3773939
245 1 0 $a Grand Canonical Approach to Modeling Dynamic Catalysts: From Thermal to Electro-Catalysis, From Clusters to Surfaces.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2024
300 $a 284 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
500 $a Advisor: Alexandrova, Anastassia N.
502 $a Thesis (Ph.D.)--University of California, Los Angeles, 2024.
520 $a Dynamic structural rearrangement has been observed in a wide range of heterogeneous catalysts and functional materials when they are in operation. Such fluxional behaviors underlie the reactivity, activation, or deactivation in various catalytic systems. However, experimentally resolving their atomic structures has been challenging due to the transient and minority nature of the metastable motifs and surface phases. The role of theory in investigating those dynamic systems hence remains singular.This dissertation will focus on the development and application of a grand canonical (GC) approach to model catalysts that undergo significant off-stoichiometric restructurings in reaction conditions. Grand canonical genetic algorithm (GCGA), an efficient global optimization algorithm, is implemented and used to explore the vast chemical space of cluster isomerization, surface atoms rearrangement, mixed coverage and configuration of adsorbates, and to locate the global and relevant local minima. The found minima constitute a GC ensemble of catalyst states that are diverse in structure, stoichiometry, and reactivity. By ab initio thermodynamics and grand canonical density functional theory (GC-DFT) calculations, the dependence on reaction conditions (temperature, partial pressures, pH, electrode potential, solute concentrations, etc.) can be included into the free energetics of the states, to probe how the distribution of states responds to varying conditions.This approach has been applied to investigate multiple systems ranging from thermal to electro-catalysis, and from supported clusters to extended surfaces. This talk will cover a few representative systems, including boron nitride in thermal oxidative dehydrogenation conditions, supported sub-nanometer metal clusters in electrocatalysis, and copper electrodes in electroreduction conditions. The dissertation works will illustrate how the GC approach not only helps interpret complex experimental observations, but also provides rich atomic insights into the structure and reactivity of catalytic species, and lays the foundation to build a new paradigm for reaction kinetics, catalyst optimization, non-equilibrium behaviors, and more.
590 $a School code: 0031.
650 4 $a Computational chemistry. $3 3350019
650 4 $a Condensed matter physics. $3 3173567
650 4 $a Materials science. $3 543314
650 4 $a Physical chemistry. $3 1981412
653 $a Catalysis
653 $a Density functional theory
653 $a Electrochemistry
653 $a Global optimization
653 $a Statistical mechanics
690 $a 0219
690 $a 0794
690 $a 0611
690 $a 0494
710 2 $a University of California, Los Angeles. $b Chemistry 0153. $3 2096181
773 0 $t Dissertations Abstracts International $g 85-11B.
790 $a 0031
791 $a Ph.D.
792 $a 2024
793 $a English
856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31296762