Recent advances in the development of single atom catalysts for oxygen evolution reaction

International Journal of Hydrogen Energy, Год журнала: 2024, Номер 82, С. 1081 - 1100

Опубликована: Авг. 9, 2024

Язык: Английский

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Hydrogen and oxygen evolution reactions on single atom catalysts stabilized by a covalent organic framework

Energy Advances, Год журнала: 2023, Номер 2(7), С. 1022 - 1029

Опубликована: Янв. 1, 2023

Catalytic activity for HER and OER of SAC made by TM atoms embedded in COF were investigated. They often form stable unconventional intermediates, these species can be more than classical adducts.

Язык: Английский

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Importance of the Walden Inversion for the Activity Volcano Plot of Oxygen Evolution

Advanced Science, Год журнала: 2023, Номер 10(36)

Опубликована: Окт. 30, 2023

Abstract Since the birth of computational hydrogen electrode approach, it is considered that activity trends electrocatalysts in a homologous series can be quantified by construction volcano plots. This method aims to steer materials discovery identification catalysts with an improved reaction kinetics, though evaluated means thermodynamic descriptors. The conventional approach for plot oxygen evolution (OER) relies on assumption mononuclear mechanism, comprising * OH, O, and OOH intermediates. In present manuscript, two new mechanistic pathways, idea Walden inversion bond‐breaking bond‐making occurs simultaneously, are factored into potential‐dependent OER plot. Surprisingly, turns out plays important role since governed pathways steps rather than traditionally assumed mechanisms under typical conditions.

Язык: Английский

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Key Ingredients for the Screening of Single Atom Catalysts for the Hydrogen Evolution Reaction: The Case of Titanium Nitride

Small, Год журнала: 2024, Номер unknown

Опубликована: Апрель 26, 2024

Abstract A computational screening of Single Atom Catalysts (SACs) bound to titanium nitride (TiN) is presented, for the Hydrogen Evolution Reaction (HER), based on density functional theory. The role fundamental ingredients explored account a reliable SACs. Namely, formation H 2 ‐complexes besides classical * one impacts predicted HER activity, in line with previous studies other Also, results indicate that needs adopt self‐interaction‐corrected functionals. Finally, predicting an active catalyst little help without assessment its stability. Thus, it included theoretical framework analysis stability SACs working conditions pH and voltage. Once unconventional intermediates are considered self‐interaction corrected scheme, number potential good catalysts strongly reduced since i) some potentially not stable against dissolution ii) leads thermodynamic barriers. This study highlights importance including prediction new systems, such as intermediates, estimating SACs, adoption this interesting candidates deserving dedicated work.

Язык: Английский

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Computationally screening non-precious single atom catalysts for oxygen reduction in alkaline media

Catalysis Today, Год журнала: 2024, Номер 431, С. 114560 - 114560

Опубликована: Фев. 3, 2024

The performance of single-atom catalysts (SACs) containing Sc, Ti, V, Mn, Fe, Ni, Cu, and Pt on N-doped carbon (NC) as possible cathodes in advanced chlor-alkali electrolysis has been investigated by means density functional theory (DFT) with the aim finding candidates to improve sluggish kinetics oxygen reduction reaction (ORR). A plausible mechanism is proposed for ORR that allows making use computational hydrogen electrode (CHE) approach this environment, suitable models have used estimate free-energy changes corresponding elementary steps. different analyzed terms electrochemical-step symmetry index (ESSI) Gmax descriptors. From these descriptors, Cu-containing SAC predicted exhibit highest catalytic activity which consistent a theoretical overpotential 0.71 V vs. standard (SHE) only, indicating type depolarized (ODCs) may overcome limitations high cost low abundance other precious metals.

Язык: Английский

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Water Splitting on a Pt1/C3N4 Single Atom Catalyst: A Modeling Approach

Topics in Catalysis, Год журнала: 2023, Номер 66(15-16), С. 1120 - 1128

Опубликована: Март 21, 2023

Abstract In this work we present a computational study of the nature Single Atom Catalyst (SAC) consisting Pt 1 atom anchored on C 3 N 4 support, and its reactivity in water splitting semi-reactions, Hydrogen Evolution (HER) Oxygen (OER) Reactions. The is motivated by intense research designing catalytic materials for characterized low amount noble metal species, maximization active phase, stability catalyst. -based SACs are promising candidates. results indicate that chemistry single complex, as it can be to support different ways resulting stability. most stable structure HER OER has been considered, finding @C more reactive than metallic platinum. Furthermore, unconventional but intermediates form differ from usually found extended surfaces. highlights importance considering complex view analogies existing with coordination compounds.

Язык: Английский

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New scaling relationships for the oxygen evolution reaction on single atom catalysts

Catalysis Today, Год журнала: 2023, Номер 427, С. 114409 - 114409

Опубликована: Окт. 14, 2023

Single Atom Catalysis is relatively new frontier in catalysis with potential application several critical chemical processes, such as water splitting reactions. atom catalysts (SACs) are analogues of coordination chemistry compounds, opening the way to formation unconventional intermediates compared extended metal or oxide catalyst surfaces. In this work we show by means density functional theory (DFT) calculations that adsorbates on SACs oxygen evolution reaction (OER) leads complex scaling relationships, differ from relations observed The evidence directly impacts expected catalytic activity and provides a further example importance including modelling species beyond those form classical electrodes.

Язык: Английский

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Giving New Life to Waste Cigarette Butts: Transformation into Platinum Group Metal-Free Electrocatalysts for Oxygen Reduction Reaction in Acid, Neutral and Alkaline Environment

Catalysts, Год журнала: 2023, Номер 13(3), С. 635 - 635

Опубликована: Март 22, 2023

Following the core theme of a circular economy, novel strategy to upcycle cigarette butt waste into platinum group metal (PGM)-free nitrogen carbon (M-N-C) electrocatalysts for oxygen reduction reaction (ORR) is presented. The experimental route was composed (i) transformation powdered butts carbonaceous char via pyrolysis at 450 °C, 600 750 °C and 900 (ii) porosity activation with KOH (iii) functionalization activated chars iron (II) phthalocyanine (FePc). electrochemical outcomes obtained by rotating disk electrode (RRDE) technique revealed that sample pyrolyzed (i.e., cig_450) outperformed other counterparts its highest onset (Eon) half-wave potentials (E1/2) demonstrated nearly tetra-electronic ORR in acidic, neutral alkaline electrolytes, all resulting from optimal surface chemistry textural properties.

Язык: Английский

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Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Advanced Theory and Simulations, Год журнала: 2024, Номер 7(9)

Опубликована: Июль 1, 2024

Abstract The electrochemical nitrogen reduction reaction (NRR) is a key process for the energy transition. Transition metal atoms atomically dispersed on solid support represent promising approach to design of new catalytic materials. interest single‐ (SACs) and dual‐atom catalysts (DACs) steadily growing. In general, DACs are considered more active than SACs NRR. this work, complex chemistry behind NRR investigated set by means density functional theory (DFT) calculations. results indicate that self‐interaction corrected exchange‐correlation functionals must be adopted, at variance with several studies in literature. Furthermore, it not possible extrapolate obtained conventional extended surfaces DACs, due richer scenario paths. show positive effect activity moving from 3d 5d metals, DACs. However, if two effects work together, is, metals intermediates may too strongly bound, thus resulting reduced activity. respect, fact expected superior always verified.

Язык: Английский

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CO2 electroreduction on single atom catalysts: Role of the local coordination

Electrochimica Acta, Год журнала: 2024, Номер 499, С. 144714 - 144714

Опубликована: Июль 15, 2024

Single Atom Catalysts (SACs) are a new frontier in catalysis, merging the positive aspects of both homogeneous and heterogenous catalysts. CO2 electrochemical reduction is key reaction for energy transition. In this work, we investigate role local coordination on activation SACs, by means density functional theory (DFT) calculations. We scrutinize 20 transitional metal atoms embedded graphene support. The results indicate that has critical to binding support CO2. environment around active site as important nature atom. At same time, stability intermediates strongly depends coordination. some cases, relative changes function environment, affecting selectivity reaction. This study provides evidence importance single-atom crucial aspect if one interested providing rationale reactivity, or predicting novel

Язык: Английский

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