Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites
Diatomic-site catalysts (DASCs) inherit the excellent performance of single-atom catalysts (SACs) by utilizing two adjacent atomic metal species to achieve functional complementarity and synergistic effects that improve the carbon dioxide reduction reaction (CO2RR) and H2 evolution reaction (HER) kinetics. Herein, we report a method to further improve the catalytic efficiency of Pt by using Pt and Ru single atoms randomly anchored on a g-C3N4 surface, yielding partial Pt-Ru dimers. The synthesized catalyst exhibits extraordinary photocatalytic activity and stability in both the CO2RR and HER processes. In-depth experimentation, the pH-dependent chemical exchange saturation transfer (CEST) imaging nuclear magnetic resonance (NMR) method, and theoretical analyses reveal that the excellent performance is attributed to orbital coupling between the Pt atoms and the neighboring Ru atoms (mainly dxy and dxz), which decreases the orbital energy levels and weakens the bond strength with intermediates, resulting in improved CO2RR and HER performance. This study successfully applies the pH-dependent CEST imaging NMR method to catalytic reactions, and CO2 adsorption is directly observed using CEST 2D imaging maps. This work presents significant potential for a variety of catalytic reaction applications by systematically designing bimetallic dimers with higher activity and stability.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:18 |
|---|---|
| Enthalten in: |
ACS nano - 18(2024), 13 vom: 02. Apr., Seite 9403-9412 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
You, Xiao-Meng [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
CO2 reduction reaction |
|---|
| Anmerkungen: |
Date Revised 02.04.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1021/acsnano.3c10807 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM369778782 |
|---|
| LEADER | 01000caa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM369778782 | ||
| 003 | DE-627 | ||
| 005 | 20240403000502.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 240315s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1021/acsnano.3c10807 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1361.xml |
| 035 | |a (DE-627)NLM369778782 | ||
| 035 | |a (NLM)38488193 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a You, Xiao-Meng |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites |
| 264 | 1 | |c 2024 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Revised 02.04.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Diatomic-site catalysts (DASCs) inherit the excellent performance of single-atom catalysts (SACs) by utilizing two adjacent atomic metal species to achieve functional complementarity and synergistic effects that improve the carbon dioxide reduction reaction (CO2RR) and H2 evolution reaction (HER) kinetics. Herein, we report a method to further improve the catalytic efficiency of Pt by using Pt and Ru single atoms randomly anchored on a g-C3N4 surface, yielding partial Pt-Ru dimers. The synthesized catalyst exhibits extraordinary photocatalytic activity and stability in both the CO2RR and HER processes. In-depth experimentation, the pH-dependent chemical exchange saturation transfer (CEST) imaging nuclear magnetic resonance (NMR) method, and theoretical analyses reveal that the excellent performance is attributed to orbital coupling between the Pt atoms and the neighboring Ru atoms (mainly dxy and dxz), which decreases the orbital energy levels and weakens the bond strength with intermediates, resulting in improved CO2RR and HER performance. This study successfully applies the pH-dependent CEST imaging NMR method to catalytic reactions, and CO2 adsorption is directly observed using CEST 2D imaging maps. This work presents significant potential for a variety of catalytic reaction applications by systematically designing bimetallic dimers with higher activity and stability | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a CO2 reduction reaction | |
| 650 | 4 | |a chemical exchange saturation transfer (CEST) imaging | |
| 650 | 4 | |a heteronuclear biatomic atom | |
| 650 | 4 | |a photocatalysis | |
| 650 | 4 | |a water splitting | |
| 700 | 1 | |a Xu, Beibei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Hang |e verfasserin |4 aut | |
| 700 | 1 | |a Qiao, Hongwei |e verfasserin |4 aut | |
| 700 | 1 | |a Lv, Xingxi |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Zejiang |e verfasserin |4 aut | |
| 700 | 1 | |a Pang, Jingyi |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Lingyun |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Peng Fei |e verfasserin |4 aut | |
| 700 | 1 | |a Guan, Xiaohong |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Hua Gui |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Xuelu |e verfasserin |4 aut | |
| 700 | 1 | |a Yao, Ye-Feng |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t ACS nano |d 2007 |g 18(2024), 13 vom: 02. Apr., Seite 9403-9412 |w (DE-627)NLM18248100X |x 1936-086X |7 nnns |
| 773 | 1 | 8 | |g volume:18 |g year:2024 |g number:13 |g day:02 |g month:04 |g pages:9403-9412 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/acsnano.3c10807 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 18 |j 2024 |e 13 |b 02 |c 04 |h 9403-9412 | ||