Rational Design of p-Block Metal-Doped Bismuth via Dual Orbital Hybridizations for Ampere-Level CO2-to-Formate Electrosynthesis and Zn-CO2 Batteries

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F25%3A10258672" target="_blank" >RIV/61989100:27740/25:10258672 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/00216208:11320/25:10504741

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/acscatal.5c05753?src=getftr&utm_source=clarivate&getft_integrator=clarivate" target="_blank" >https://pubs.acs.org/doi/10.1021/acscatal.5c05753?src=getftr&utm_source=clarivate&getft_integrator=clarivate</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.5c05753" target="_blank" >10.1021/acscatal.5c05753</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Rational Design of p-Block Metal-Doped Bismuth via Dual Orbital Hybridizations for Ampere-Level CO2-to-Formate Electrosynthesis and Zn-CO2 Batteries

Popis výsledku v původním jazyce

Electrochemical conversion of CO2 into formate stands as a compelling pathway toward carbon neutrality, where the attainment of high selectivity under industrial-current-density electrolysis conditions represents a pivotal milestone toward scalable implementation. In this work, dual orbital hybridizations (s-p hybridization of Sn 5s and O 2p orbitals and p-p hybridization of Sn 5p/Bi 6p and O 2p orbitals) are introduced to synergistically regulate charge transfer dynamics between active sites and oxygenated intermediates via integrating p-block metals into bismuth nanosheets. The resulting Sn-doped Bi catalyst (Sn1Bi) achieved a record-breaking partial current density of -2.56 A cm(-2) for formate production, sustaining 85.4% Faradaic efficiency even at -3 A cm(-2), along with an unprecedented robustness at 2 A for 280 h in a membrane electrode assembly. Ongoing mechanistic studies aim to elucidate that dual orbital hybridizations facilitate CO2 activation and stabilize the critical *OCHO intermediate, thereby optimizing reaction kinetics and formate selectivity. This study advances the rational design of dual p-p and s-p orbital hybridization-engineered electrocatalysts for the selective and efficient valorization of CO2.

Název v anglickém jazyce

Rational Design of p-Block Metal-Doped Bismuth via Dual Orbital Hybridizations for Ampere-Level CO2-to-Formate Electrosynthesis and Zn-CO2 Batteries

Popis výsledku anglicky

Electrochemical conversion of CO2 into formate stands as a compelling pathway toward carbon neutrality, where the attainment of high selectivity under industrial-current-density electrolysis conditions represents a pivotal milestone toward scalable implementation. In this work, dual orbital hybridizations (s-p hybridization of Sn 5s and O 2p orbitals and p-p hybridization of Sn 5p/Bi 6p and O 2p orbitals) are introduced to synergistically regulate charge transfer dynamics between active sites and oxygenated intermediates via integrating p-block metals into bismuth nanosheets. The resulting Sn-doped Bi catalyst (Sn1Bi) achieved a record-breaking partial current density of -2.56 A cm(-2) for formate production, sustaining 85.4% Faradaic efficiency even at -3 A cm(-2), along with an unprecedented robustness at 2 A for 280 h in a membrane electrode assembly. Ongoing mechanistic studies aim to elucidate that dual orbital hybridizations facilitate CO2 activation and stabilize the critical *OCHO intermediate, thereby optimizing reaction kinetics and formate selectivity. This study advances the rational design of dual p-p and s-p orbital hybridization-engineered electrocatalysts for the selective and efficient valorization of CO2.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

Návaznosti

—

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ACS Catalysis

ISSN

2155-5435

e-ISSN

2155-5435

Svazek periodika

15

Číslo periodika v rámci svazku

21

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

18525-18534

Kód UT WoS článku

001600446800001

EID výsledku v databázi Scopus

—