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

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Expanding the frontiers of electrocatalysis: advanced theoretical methods for water splitting

Nano Convergence, Год журнала: 2025, Номер 12(1)

Опубликована: Янв. 24, 2025

Abstract Electrochemical water splitting, which encompasses the hydrogen evolution reaction (HER) and oxygen (OER), offers a promising route for sustainable production. The development of efficient cost-effective electrocatalysts is crucial advancing this technology, especially given reliance on expensive transition metals, such as Pt Ir, in traditional catalysts. This review highlights recent advances design optimization electrocatalysts, focusing density functional theory (DFT) key tool understanding improving catalytic performance HER OER. We begin by exploring DFT-based approaches evaluating activity under both acidic alkaline conditions. then shifts to material-oriented perspective, showcasing catalyst materials theoretical strategies employed enhance their performance. In addition, we discuss scaling relationships that exist between binding energies electronic structures through use charge-density analysis d -band theory. Advanced concepts, effects adsorbate coverage, solvation, applied potential behavior, are also discussed. finally focus integrating machine learning (ML) with DFT enable high-throughput screening accelerate discovery novel water-splitting comprehensive underscores pivotal role plays electrocatalyst its shaping future Graphical

Язык: Английский

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Dual‐Shelled Hollow Leafy Carbon Support with Atomically Dispersed (N,S)‐Bridged Hydroxy‐Coordinated Asymmetric Fe Sites for Oxygen Reduction

Advanced Functional Materials, Год журнала: 2024, Номер 34(29)

Опубликована: Апрель 21, 2024

Abstract Single‐atom catalysts (SACs) are widely studied in various chemical transformations due to their high catalytic activity and atom utilization. However, modulating the performance of by adjusting microenvironment remains a great challenge. In this paper, novel master‐double guest vulcanization‐assisted strategy is reported for synthesizing Fe single‐atom on N,S codoped porous hollow leaf carbon (Fe SA /N,S‐PHLC) with highly exposed FeN 3 SOH sites. Fe(mIm) (guest I) loaded surface ZIF‐L (host) then trithiocyanuric acid (TCA, II) bonded Fe(mIm), resulting ZIF‐L@Fe(mIm)@TCA precursors can be converted /N,S‐PHLC controllable structures. addition, XPS analysis yield an increase pyridine N content compared /N‐PHLC. It demonstrated theoretical calculations that N,S‐coordinated axially hydroxy‐coordinated asymmetric centers synergistically abundance pyridinic nitrogen facilitate adsorption desorption oxygen intermediates, 3d orbitals active optimized. The prepared catalyst has half‐wave potential (E 1/2 ) 0.91 V under alkaline conditions, E = 0.75 acidic conditions. shows excellent cycle stability (882 h) power density (217 mW cm −2 assembly zinc–air battery (ZABs) devices.

Язык: Английский

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Theoretical Calculation Assisted by Machine Learning Accelerate Optimal Electrocatalyst Finding for Hydrogen Evolution Reaction

ChemElectroChem, Год журнала: 2024, Номер 11(13)

Опубликована: Апрель 11, 2024

Abstract Electrocatalytic hydrogen evolution reaction (HER) is a promising strategy to solve and mitigate the coming energy shortage global environmental pollution. Searching for efficient electrocatalysts HER remains challenging through traditional trial‐and‐error methods from numerous potential material candidates. Theoretical high throughput calculation assisted by machine learning possible method screen excellent effectively. This will pave way high‐efficiency low‐price electrocatalyst findings. In this review, we comprehensively introduce workflow standard models reduction reactions. mainly illustrates how used in catalyst filtration descriptor exploration. Subsequently, several applications, including surface electrocatalysts, two‐dimensional (2D) single/dual atom using electrocatalytic HER, are highlighted introduced. Finally, corresponding challenge perspective reactions concluded. We hope critical review can provide comprehensive understanding of design guide future theoretical experimental investigation

Язык: Английский

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Recent Advances for Seawater Hydrogen Evolution

ChemCatChem, Год журнала: 2024, Номер 16(14)

Опубликована: Янв. 23, 2024

Abstract Hydrogen production from electrolysis of seawater is considered one the most promising endeavors. However, complexity environment (corrosion‐prone, slow kinetics, and side reactions such as precipitation generation) leaves much room for progress in research on efficient stable catalysts. In recent years, order to improve technology hydrogen electrolytic seawater, scientists have focused preparation catalysts design electrolytes, which has resulted important progress. further understand current status development prospects evolution reaction (HER), this article summarizes general rules electrocatalysts electrolytes HER years. For structure modulation, effects catalyst modulation strategies heterostructures, elemental doping, manufacturing defects, morphology engineering others performance enhancement are highlighted. Overall guidelines summarized electrolyte directions future in‐depth exploration proposed with a view early realization an industrial scale.

Язык: Английский

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CuCo DAC used to change the hydrogenation sequence for efficient electrochemical C-N coupling

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 351, С. 124003 - 124003

Опубликована: Апрель 24, 2024

Язык: Английский

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Collaborative Interface Optimization Strategy Guided Fe3C/MnO-NC Electrocatalysts for Rechargeable Flexible Zinc-Air Batteries

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер unknown, С. 124615 - 124615

Опубликована: Сен. 1, 2024

Язык: Английский

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Hydrogenated Pyridine‐Pyrrole Nitrogen‐Doped Carbon for High‐Efficiency Electrosynthesis of Hydrogen Peroxide in NaCl Electrolyte

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 26, 2024

Abstract Developing metal‐free carbon catalysts is critical to achieve the electrosynthesis of hydrogen peroxide (H 2 O ) via two‐electron oxygen reduction reaction (2e − ORR) using seawater as electrolyte. Herein, N‐rich doped (NC) synthesized by directly pyrolyzing guanine both N and C sources, which can facilitate formation ultrahigh‐N dopant (up 33.89 at.%), their ratios. The NC obtained at 700 °C with hydrogenated pyridine‐N pyrrole‐N (3:2) dopants exhibits a superior selectivity H 96%), high mass activity 545.5 A g −1 0.2 V versus RHE stable production 16.8 in 0.5 M NaCl. In situ Fourier transform infrared spectrum analysis proves that play role constructing active sites for synthesis . Meanwhile, theoretical calculations further reveal compared non‐hydrogenated dopants, pyridine pyrrole tune projected density states 2p z orbitals adjacent atoms approaching Fermi Level, enhancing * OOH through 2e ORR rather than 4e ORR. This work provides new insights developing efficient resources promising electrolytes.

Язык: Английский

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Coaxial Metal‐Nitrogen–Carbon Single‐Atom Catalysts Boost Acid Hydrogen Peroxide Production

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Дек. 10, 2024

Abstract Electrosynthesis of hydrogen peroxide (H 2 O ) by two‐electron oxygen reduction reaction (2e − ORR) under acidic conditions is promising. However, constructing a highly efficient acid‐resistant 2e ORR electrocatalyst critical but challenging. Herein, coaxial cobalt single‐atom catalyst on carbon nanotubes (Co SA ‐N‐C/CNTs) designed and synthesized an ingenious separation chemical vapor deposition (SCVD) strategy, which achieves higher activity, dominated selectivity, superior stability in acid, compared to the counterpart nanoparticle prepared traditional mixture pyrolysis. The as‐assembled electrode using Co ‐N‐C/CNTs demonstrates high H yield excess 2000 mmol g cat −1 h with Faraday efficiency >90% over 100 without decay flow cell, as most reported production catalysts. Experimental characterization theoretical calculations reveal that such excellent performance originate from combined advantages strongly coupled core–shell structure dispersed property. Most importantly, series other transition metal catalysts (M ‐N‐C/CNTs, M = Fe, Cu, or Ni) are through this SCVD they all show enhanced performance, demonstrating universality.

Язык: Английский

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Oxidative dehydrogenation of ethylbenzene on mesoporous carbon catalysts: effect of the active site number on the apparent catalytic activity

Catalysis Science & Technology, Год журнала: 2024, Номер 14(6), С. 1550 - 1557

Опубликована: Янв. 1, 2024

SMC- x catalysts demonstrate a distinctive carbon framework containing significant number of CO active sites for ethylbenzene oxidative dehydrogenation.

Язык: Английский

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