Sustainable zinc–air battery chemistry: advances, challenges and prospects

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6139 - 6190

Published: Jan. 1, 2023

Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted addressing the critical challenges associated with sustainable ZABs, aiming significantly improve efficiency and prolong operation lifespan. The growing interest in ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, Zn anodes, which not systematically reviewed date. In this review, fundamentals of electrocatalysts air cathodes, physicochemical properties ZAB issues strategies stabilization anodes summarized from perspective fundamental characteristics design principles. Meanwhile, significant advances situ/operando characterization highlighted provide insights into reaction mechanism dynamic evolution electrolyte|electrode interface. Finally, several thoughts perspectives provided regarding opportunities ZABs. Therefore, review provides a thorough understanding advanced chemistry, hoping that timely comprehensive can shed light upcoming horizons prosperous area.

Language: Английский

---

Oxophilicity-Controlled CO₂ Electroreduction to C₂₊ Alcohols over Lewis Acid Metal-Doped Cu^δ+ Catalysts

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(40), P. 21945 - 21954

Published: Sept. 26, 2023

Cu-based electrocatalysts have great potential for facilitating CO2 reduction to produce energy-intensive fuels and chemicals. However, it remains challenging obtain high product selectivity due the inevitable strong competition among various pathways. Here, we propose a strategy regulate adsorption of oxygen-associated active species on Cu by introducing an oxophilic metal, which can effectively improve C2+ alcohols. Theoretical calculations manifested that doping Lewis acid metal Al into affect C–O bond Cu–C breaking toward selectively determining intermediate (shared ethanol ethylene), thus prioritizing pathway. Experimentally, Al-doped catalyst exhibited outstanding Faradaic efficiency (FE) 84.5% with remarkable stability. In particular, alcohol FE could reach 55.2% partial current density 354.2 mA cm–2 formation rate 1066.8 μmol h–1. A detailed experimental study revealed improved strength oxygen surface stabilized key *OC2H5, leading ethanol. Further investigation showed this also be extended other metals.

Language: Английский

---

Cooperation between Dual Metal Atoms and Nanoclusters Enhances Activity and Stability for Oxygen Reduction and Evolution

ACS Nano, Journal Year: 2023, Volume and Issue: 17(9), P. 8622 - 8633

Published: April 27, 2023

We have achieved the synthesis of dual-metal single atoms and atomic clusters that co-anchor on a highly graphitic carbon support. The catalyst comprises Ni4 (and Fe4) nanoclusters located adjacent to corresponding NiN4 FeN4) single-atom sites, which is verified by systematic X-ray absorption characterization density functional theory calculations. A distinct cooperation between Fe4 (Ni4) FeN4 (NiN4) sites optimizes adsorption energy reaction intermediates reduces barrier potential-determining steps. This exhibits enhanced oxygen reduction evolution activity long-cycle stability compared counterparts without commercial Pt/C. fabricated Zn-air batteries deliver high power long-term cyclability, demonstrating their prospects in storage device applications.

Language: Английский

---

Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 5500 - 5512

Published: Jan. 1, 2023

Tb 2 O 3 endows Co 3d with a narrow band and appropriate location via 3d–O 2p–Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.

Language: Английский

---

Recent Advances in Non‐Precious Metal Single‐Atom Electrocatalysts for Oxygen Reduction Reaction in Low‐Temperature Polymer‐Electrolyte Fuel Cells

ChemCatChem, Journal Year: 2023, Volume and Issue: 15(22)

Published: Oct. 9, 2023

Abstract Fuel cells have emerged as a promising clean electrochemical energy technology with great potential in various sectors, including transportation and power generation. However, the high cost scarcity of noble metals currently used to synthesise electrocatalysts for low‐temperature fuel has hindered their widespread commercialisation. In recent decades, development non‐precious metal cathodic oxygen reduction reaction (ORR) gained significant attention. Among those, atomically dispersed active sites, referred single‐atom catalysts (SACs), are gaining more interest. Nanocarbon materials containing single transition atoms coordinated nitrogen ORR both acidic alkaline conditions thus promise be utilised cathode cells. This review article provides an overview advancements utilisation metal‐based SACs proton exchange membrane (PEMFCs) anion (AEMFCs). We highlight main strategies synthetic approaches tailoring properties enhance activity durability. Based on already achieved results, it is evident that indeed could suitable

Language: Английский

---

Microwave‐Assisted Rapid Synthesis of MOF‐Based Single‐Atom Ni Catalyst for CO₂ Electroreduction at Ampere‐Level Current

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 17, 2024

Carbon-based single-atom catalysts (SACs) have attracted tremendous interest in heterogeneous catalysis. However, the common electric heating techniques to produce carbon-based SACs usually suffer from prolonged time and tedious operations. Herein, a general facile microwave-assisted rapid pyrolysis method is developed afford within 3 min without inert gas protection. The obtained present high porosity comparable carbonization degree those by techniques. Specifically, Ni implanted N-doped carbon (Ni

Language: Английский

---

Highly Reversible Zn–Air Batteries Enabled by Tuned Valence Electron and Steric Hindrance on Atomic Fe–N₄–C Sites

Nano Letters, Journal Year: 2024, Volume and Issue: 24(15), P. 4672 - 4681

Published: April 8, 2024

The bifunctional oxygen electrocatalyst is the Achilles' heel of achieving robust reversible Zn–air batteries (ZABs). Herein, durable electrocatalysis in alkaline media realized on atomic Fe–N4–C sites reinforced by NixCo3–xO4 (NixCo3–xO4@Fe1/NC). Compared with that pristine Fe1/NC, stability evolution reaction (OER) increased 10 times and reduction (ORR) performance also improved. steric hindrance alters valence electron at sites, resulting a shorter Fe–N bond enhanced sites. corresponding solid-state ZABs exhibit an ultralong lifespan (>460 h 5 mA cm–2) high rate (from 2 to 50 cm–2). Furthermore, structural NixCo3–xO4@Fe1/NC before after OER ORR as well charge–discharge cycling explored. This work develops efficient strategy for improving possibly other processes.

Language: Английский

---

Collective Effect in a Multicomponent Ensemble Combining Single Atoms and Nanoparticles for Efficient and Durable Oxygen Reduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 13, 2024

Abstract Metal single‐atom catalysts represent one of the most promising non‐noble metal for oxygen reduction reaction (ORR). However, they still suffer from insufficient activity and, particularly, durability practical applications. Leveraging density functional theory (DFT) and machine learning (ML), we unravel an unexpected collective effect between FeN 4 OH sites, CeN motifs, Fe nanoparticles (NPs), Fe−CeO 2 NPs. The comprises differently‐weighted electronic geometric interactions, whitch results in significantly enhanced ORR active sites with a half‐wave potential ( E 1/2 ) 0.948 V versus reversible hydrogen electrode (V RHE alkaline, relative to commercial Pt/C , 0.851 ). Meanwhile, this endows shortened Fe−N bonds remarkable negligible loss after 50,000 cycles. ML was used understand intricate interactions reveal intrinsic descriptors account performance. universality demonstrated effective Co, Ni, Cu, Cr, Mn‐based multicomponent ensembles. These confirm importance simultaneously improve catalytic durability.

Language: Английский

---

Revealing the Active Sites in Atomically Dispersed Multi‐Metal–Nitrogen–Carbon Catalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: Jan. 30, 2024

Abstract Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these are likely to consist of combination single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained challenging task. In this study, model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom CoMn on nitrogen‐doped carbon substrate. By employing X‐ray adsorption spectroscopy density functional theory calculations, the atomic configuration Co/CoMn‐NC determined. Density calculations also used unequivocally identify Co‐atom within motif as predominate site toward oxygen reduction reaction (ORR), which further confirmed by in situ Raman spectroscopy. The cooperative interactions between can finely tune d‐band center ameliorate desorption behaviors intermediates, thereby facilitating ORR kinetic. Overall, study introduces systematic strategy elucidate structure superiority system provides new insights into atomically multi‐metal sites, showcasing that enhanced catalytic performance extends beyond unified diatomic or monatomic

Language: Английский

---

Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

---