Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216305%3A26620%2F24%3APU150704" target="_blank" >RIV/00216305:26620/24:PU150704 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989592:15310/24:73622693

Výsledek na webu

<a href="https://onlinelibrary.wiley.com/doi/10.1002/smll.202304574" target="_blank" >https://onlinelibrary.wiley.com/doi/10.1002/smll.202304574</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/smll.202304574" target="_blank" >10.1002/smll.202304574</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol

Popis výsledku v původním jazyce

Direct selective transformation of greenhouse methane (CH4) to liquid oxygenates (methanol) can substitute energy-intensive two-step (reforming/Fischer-Tropsch) synthesis while creating environmental benefits. The development of inexpensive, selective, and robust catalysts that enable room temperature conversion will decide the future of this technology. Single-atom catalysts (SACs) with isolated active centers embedded in support have displayed significant promises in catalysis to drive challenging reactions. Herein, high-density Ni single atoms are developed and stabilized on carbon nitride (NiCN) via thermal condensation of preorganized Ni-coordinated melem units. The physicochemical characterization of NiCN with various analytical techniques including HAADF-STEM and X-ray absorption fine structure (XAFS) validate the successful formation of Ni single atoms coordinated to the heptazine-constituted CN network. The presence of uniform catalytic sites improved visible absorption and carrier separation in densely populated NiCN SAC resulting in 100% selective photoconversion of (CH4) to methanol using H2O2 as an oxidant. The superior catalytic activity can be attributed to the generation of high oxidation (NiIIIO) sites and selective CH bond cleavage to generate center dot CH3 radicals on Ni centers, which can combine with center dot OH radicals to generate CH3OH. Performing selective photooxidation of methane into methanol under visible light using an inexpensive and robust Ni single atom catalysts. The catalyst synthesis involves two steps: i) nickel complexation with melem units; ii) thermal condensation. Melem units prevent the probability of metal coarsening during thermal treatment generating unsymmetrical tetra-coordinated Ni-N4 sites embedded in the heptazine cavity.image

Název v anglickém jazyce

Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol

Popis výsledku anglicky

Direct selective transformation of greenhouse methane (CH4) to liquid oxygenates (methanol) can substitute energy-intensive two-step (reforming/Fischer-Tropsch) synthesis while creating environmental benefits. The development of inexpensive, selective, and robust catalysts that enable room temperature conversion will decide the future of this technology. Single-atom catalysts (SACs) with isolated active centers embedded in support have displayed significant promises in catalysis to drive challenging reactions. Herein, high-density Ni single atoms are developed and stabilized on carbon nitride (NiCN) via thermal condensation of preorganized Ni-coordinated melem units. The physicochemical characterization of NiCN with various analytical techniques including HAADF-STEM and X-ray absorption fine structure (XAFS) validate the successful formation of Ni single atoms coordinated to the heptazine-constituted CN network. The presence of uniform catalytic sites improved visible absorption and carrier separation in densely populated NiCN SAC resulting in 100% selective photoconversion of (CH4) to methanol using H2O2 as an oxidant. The superior catalytic activity can be attributed to the generation of high oxidation (NiIIIO) sites and selective CH bond cleavage to generate center dot CH3 radicals on Ni centers, which can combine with center dot OH radicals to generate CH3OH. Performing selective photooxidation of methane into methanol under visible light using an inexpensive and robust Ni single atom catalysts. The catalyst synthesis involves two steps: i) nickel complexation with melem units; ii) thermal condensation. Melem units prevent the probability of metal coarsening during thermal treatment generating unsymmetrical tetra-coordinated Ni-N4 sites embedded in the heptazine cavity.image

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

—

Návaznosti

—

Rok uplatnění

2024

Kód důvěrnosti údajů

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

Název periodika

Small

ISSN

1613-6810

e-ISSN

1613-6829

Svazek periodika

20

Číslo periodika v rámci svazku

15

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

12

Strana od-do

„“-„“

Kód UT WoS článku

001108786800001

EID výsledku v databázi Scopus

2-s2.0-85178261071