Orbital-Engineering-Based Screening of π-Conjugated d8 Transition-Metal Coordination Polymers for High-Performance n-Type Thermoelectric Applications.
ACS Appl Mater Interfaces
; 10(41): 35306-35315, 2018 Oct 17.
Article
em En
| MEDLINE
| ID: mdl-30251818
Extraordinary progress has been achieved in polymer-based thermoelectric materials in recent years. New emerging π-conjugated transition-metal coordination polymers are one of the best n-type polymer-based thermoelectric materials. However, the microscopic descriptions on geometric structures, orbital characteristics, and most importantly, thermoelectric properties remain elusive, which has seriously hampered the experimentalists to draw a straightforward design strategy for new n-type polymer-based thermoelectric materials. Herein, we assess the n-type thermoelectric properties of 20 π-conjugated d8 metal center coordination polymers and rationalize their thermoelectric properties in terms of molecular geometry, orbital nature, and electron-phonon coupling based on first-principles calculations. An explicit screening rule for high-performance n-type π-conjugated transition-metal coordination polymeric thermoelectric materials was found, i.e., smaller metal center d orbital component ratio in the conduction band minimum, weaker electron-phonon coupling, higher intrinsic mobility, and thereby higher thermoelectric power factor can be achieved. Guided by this rule, poly(Pd-C2S4) and poly(Ni-C2Se4) show very high power factors. We built a map of high-performance π-conjugated transition-metal coordination polymers for n-type thermoelectric applications, which will help to accelerate the screening and design of innovative n-type thermoelectric polymers.
Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Tipo de estudo:
Diagnostic_studies
/
Screening_studies
Idioma:
En
Revista:
ACS Appl Mater Interfaces
Assunto da revista:
BIOTECNOLOGIA
/
ENGENHARIA BIOMEDICA
Ano de publicação:
2018
Tipo de documento:
Article
País de afiliação:
Singapura
País de publicação:
Estados Unidos