Atomic Engineering of 3D Self‐Supported Bifunctional Oxygen Electrodes for Rechargeable Zinc‐Air Batteries and Fuel Cell Applications

Advanced Energy Materials, Год журнала: 2024, Номер 14(30)

Опубликована: Май 28, 2024

Abstract The oxygen evolution reaction (OER) and reduction (ORR) are cornerstone half reactions involved in many renewable energy technologies. High‐density single‐atom catalysts maximize the atom utilization isolated active sites. Furthermore, introduction of pyri‐N into carbon‐based nanostructures as an electrocatalyst creates abundance Here, innovative strategy is reported based on atomic scale dispersion Co atoms enriched carbon nanotube encapsulated Ni nanoparticles grown 3D electrospun nanofiber nano‐assemblies. Notably, SA Ni‐NCNT/CNF exhibited excellent OER ORR activity terms low overpotentials higher half‐wave potentials. atomically distributed allows maximum exposure sites dominated multidimensional skeleton, synergistic effects with greatly reduced delocalization around metal centers provided ideal environment for interactions intermediates, thus facilitating 4e − pathway, evidenced by DFT calculations. Moreover, Zn‐air batteries using a air cathode high‐power density admirable specific capacity. This studies may provide avenue rational modulation cost‐effective, large‐scale synthesis bifunctional electrocatalysts rechargeable anion exchange membrane fuel cell.

Язык: Английский

---

Unveiling Favorable Microenvironment on Porous Doped Carbon Nanosheets for Superior H₂O₂ Electrosynthesis in Neutral Media

Advanced Energy Materials, Год журнала: 2024, Номер 14(19)

Опубликована: Фев. 21, 2024

Abstract Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous to form an oxygen‐rich and local alkaline‐like microenvironment two‐electron oxygen reduction (2e − ORR) in neutral medium are designed. The situ ex test results confirmed that architecture can elevate pH accelerate generation intermediates (*O 2 , *OOH), leading high‐efficiency H O production. Utilizing this favorable microenvironment, N,O‐CNS 0.5 demonstrated exceptional electrosynthesis performance media, achieving superior yield rate (6705 mmol g catalyst −1 h flow cell). Additionally, comparative experiments density‐functional theory calculations provided confirmation bi‐doping N as active origin responsible electrochemical 2e ORR. This study synergistically manipulates sites, providing opportunity efficient electro‐production medium.

Язык: Английский

---

Atomic‐Level Engineered Cobalt Catalysts for Fenton‐Like Reactions: Synergy of Single Atom Metal Sites and Nonmetal‐Bonded Functionalities

Advanced Materials, Год журнала: 2024, Номер 36(32)

Опубликована: Апрель 30, 2024

Abstract Single atom catalysts (SACs) are atomic‐level‐engineered materials with high intrinsic activity. Catalytic centers of SACs typically the transition metal (TM)–nonmetal coordination sites, while functions coexisting non‐TM‐bonded functionalities usually overlooked in catalysis. Herein, scalable preparation carbon‐supported cobalt‐anchored (CoCN) controlled Co─N sites and free functional N species is reported. The role metal‐ nonmetal‐bonded for peroxymonosulfate (PMS)‐driven Fenton‐like reactions first systematically studied, revealing their contribution to performance improvement pathway steering. Experiments computations demonstrate that 3 C plays a vital formation surface‐confined PMS* complex trigger electron transfer promote kinetics because optimized electronic state Co centers, nonmetal‐coordinated graphitic act as preferable pollutant adsorption additional PMS activation accelerate transfer. Synergistically, CoCN exhibits ultrahigh activity p ‐hydroxybenzoic acid oxidation, achieving complete degradation within 10 min an turnover frequency 0.38 −1 , surpassing most reported materials. These findings offer new insights into versatile inspire rational design high‐performance complicated heterogeneous systems.

Язык: Английский

---

Efficient Neutral H2O2 Electrosynthesis from Favorable Reaction Microenvironments via Porous Carbon Carrier Engineering

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 20, 2024

The efficient electrosynthesis of hydrogen peroxide (H

Язык: Английский

---

Enhanced Electron Delocalization Induced by Ferromagnetic Sulfur doped C 3 N 4 Triggers Selective H 2 O 2 Production

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Май 21, 2024

For the 2D metal-free carbon catalysts, atomic coplanar architecture enables a large number of p

Язык: Английский

---

Advancing H₂O₂ electrosynthesis: enhancing electrochemical systems, unveiling emerging applications, and seizing opportunities

Chemical Society Reviews, Год журнала: 2024, Номер 53(16), С. 8137 - 8181

Опубликована: Янв. 1, 2024

Hydrogen peroxide (H

Язык: Английский

---

Unraveling the Tandem Effect of Nitrogen Configuration Promoting Oxygen Reduction Reaction in Alkaline Seawater

Advanced Energy Materials, Год журнала: 2024, Номер 14(24)

Опубликована: Апрель 10, 2024

Abstract Developing seawater‐based high‐performance oxygen reduction reaction (ORR) electrocatalysts is meaningful to renewable energy storage and conversion, the Fe‐based derivatives encapsulated by nitrogen (N) doped carbon are typical representative. Nevertheless, unrevealing mechanism of N configuration ORR activity chlorine resistance still a great challenge. In this work, feasible strategy developed prepare controllable pyridinic/pyrrolic‐N carbon‐coated (Fe x N‐NC). Drawing support from H 3 PO 4 blocking based in situ Fourier transform infrared spectroscopy (FTIR) test density‐functional theory (DFT) calculation, tandem effect pyridinic‐N pyrrolic‐N on proved. Additionally, low hydrogen peroxide (H 2 O ) yield 4e − pathway Fe N‐NC demonstrate that doping effectively reduces adsorption Cl , which consistent with DFT. The half‐wave potential (E 1/2 for reaches 0.874 V alkaline seawater, ZABs assembled as air cathode deliver remarkable power density (162 mW cm −2 ), along excellent long‐term durability (>400 h).

Язык: Английский

---

Selective oxygen reduction reaction: mechanism understanding, catalyst design and practical application

Chemical Science, Год журнала: 2024, Номер 15(29), С. 11188 - 11228

Опубликована: Янв. 1, 2024

The oxygen reduction reaction (ORR) is a key component for many clean energy technologies and other industrial processes. However, the low selectivity sluggish kinetics of ORR catalysts have hampered conversion efficiency real application these new mentioned before. Recently, tremendous efforts been made in mechanism understanding, electrocatalyst development system design. Here, comprehensive critical review provided to present recent advances field electrocatalytic ORR. two-electron four-electron transfer catalytic mechanisms evaluation parameters are discussed first. Then, up-to-date synthetic strategies

Язык: Английский

---

Surface Redox Chemistry Regulates the Reaction Microenvironment for Efficient Hydrogen Peroxide Generation

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(22), С. 15356 - 15365

Опубликована: Май 22, 2024

Electrosynthesis has emerged as an enticing solution for hydrogen peroxide (H2O2) production. However, efficient H2O2 generation encounters challenges related to the robust gas–liquid–solid interface within electrochemical reactors. In this work, we introduce effective hydrophobic coating modified by iron (Fe) sites optimize reaction microenvironment. This modification aims mitigate radical corrosion through Fe(II)/Fe(III) redox chemistry, reinforcing microenvironment at three-phase interface. Consequently, achieved a remarkable yield of up 336.1 mmol h–1 with sustained catalyst operation extensive duration 230 h 200 mA cm–2 without causing damage Additionally, Faradaic efficiency exceeded 90% across broad range test current densities. surface chemistry approach manipulating not only advances long-term electrosynthesis but also holds promise other gas-starvation reactions.

Язык: Английский

---

Accelerated O2 adsorption and stabilized *OOH for electrocatalytic H2O2 production

Journal of Material Science and Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

---