Long-Range Regulation of Se Doping for Oxygen Reduction of Atomically Dispersed Sb Catalysts for Ultralow-Temperature Solid-State Zn–Air Batteries

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(10), P. 7122 - 7131

Published: May 11, 2023

Regulating the p-orbital valence electrons of atomically dispersed main-group metals to improve inherent electrocatalytic activity has attracted extensive concerns. Herein, we designed and synthesized an Sb–SeNC catalyst containing SbN2C2 SeC2 structures, which have been identified by X-ray absorption spectroscopy density functional theory (DFT) calculations. exhibits a high for oxygen reduction reaction (ORR), Sb–SeNC-based flexible solid-state zinc–air battery (ZAB) can work efficiently at −40 °C, with peak power 54.1 mW cm–2 rate discharge operation about 44 h. DFT calculations further confirm long-range regulation mechanism moiety ORR obtain volcano relationship Uonset vs Se–N distance. When distance is 7.4 Å, adsorption ability active site Sb be regulated optimal state related RDS: *O → *OH, while smaller in short-range would lead excessive attenuation decrease activity, therefore yields effect Se doping on SbN2C2. This strategy may provide promising approach boost catalytic metal catalysts achieve its application ultralow-temperature ZABs.

Language: Английский

---

Simultaneous integration of Fe clusters and NiFe dual single atoms in nitrogen-doped carbon for oxygen reduction reaction

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 2291 - 2297

Published: Aug. 18, 2023

Language: Английский

---

Bamboo‐Modulated Helical Carbon Nanotubes for Rechargeable Zn‐Air Battery

Small, Journal Year: 2023, Volume and Issue: 20(14)

Published: Nov. 21, 2023

Abstract The high‐performance and sustainable electrocatalysts toward oxygen reduction reaction (ORR) evolution (OER) are essential for rechargeable Zn‐air batteries (ZABs). In this paper, a natural all‐components bamboo is provided as the carbon source, melamine cobalt chloride nitrogen sources, respectively. As result, unique helical nanotubes (HCNTs) encapsulated nanoparticles prepared, which acted ORR/OER to improve ZABs performance. resultant HCNTs contribute high activities via exposing more Co─N sites, providing excellent electron conductivity, facilitating mass transfer of reactant. assembled liquid showed maximum output power density 226 mW cm −2 low voltage gap 0.85 V 330 h cycles. flexible all‐solid‐state achieved with 59.4 charge–discharge cycles over 25 h. functional theory (DFT) calculations reveal that increase at effectively regulates electronic structure Co, optimizing binding affinity intermediates resulting in overpotentials. This work paves way transforming renewable biomass into versatile electrocatalysts, boosts development next‐generation energy storage conversion devices.

Language: Английский

---

Reversed I ₁ Cu ₄ single-atom sites for superior neutral ammonia electrosynthesis with nitrate

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(37)

Published: Sept. 3, 2024

Electrochemical ammonia (NH 3 ) synthesis from nitrate reduction (NITRR) offers an appealing solution for addressing environmental concerns and the energy crisis. However, most of developed electrocatalysts reduce NO − to NH via a hydrogen (H*)-mediated mechanism, which suffers undesired H*-H* dimerization H 2 , resulting in unsatisfactory yields. Herein, we demonstrate that reversed I 1 Cu 4 single-atom sites, prepared by anchoring iodine single atoms on surface, realized superior NITRR with yield rate 4.36 mg h −1 cm −2 Faradaic efficiency 98.5% under neutral conditions proton-coupled electron transfer (PCET) far beyond those traditional sites 0.082 36.5%) H*-mediated electrocatalysts. Theoretical calculations revealed can regulate local electronic structures adjacent favor stronger O-end-bidentate adsorption dual channels suppress H* formation O dissociation, thus switching mechanism PCET. By integrating monolithic electrode into flow-through device continuous situ recovery, industrial-level current density A was achieved along 69.4 . This study electrochemical wastewater sheds light importance catalytic mechanisms improving performance reactions.

Language: Английский

---

Near-range modulation of single-atomic Fe sites by simultaneously integrating heteroatom and nanocluster for efficient oxygen reduction

Nano Energy, Journal Year: 2024, Volume and Issue: 126, P. 109668 - 109668

Published: April 23, 2024

Language: Английский

---