First-row transition metal embedded pyrazine-based graphynes as high-performance single atom catalysts for the CO<sub>2</sub>reduction reaction

Wang, Maohuai; Kong, Lingyan; Lü, Xiaoqing; Wu, Lawrence

doi:10.1039/d2ta00654e

Cited by 30 publications

(13 citation statements)

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“…In this work, the DFT calculation are conducted using Vienna Ab initio Simulation Package 6.1.0 (VASP). [47][48][49] In general, the projector augmented wave (PAW) method is used to deal with electron-ion interactions, [50,51] while the Perdew-Burke Ernzerhof (PBE) exchange correlation functional is used to describe electron interactions in the generalized gradient approximation(GGA). [52] The k-point was set as 3 × 3 × 1 for geometry optimization and 11 × 11 × 1 for electronic structure computation.…”

Section: Methodsmentioning

confidence: 99%

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Lü

Cao

et al. 2023

ChemSusChem

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Single‐atom catalysts (SACs) are promising electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), in which the coordination environment plays a crucial role in activating the intrinsic activity of the central metal. Taking the FeN4 SAC as a probe, this work investigates the effect of introducing S or P atoms into N coordination (FeSxN4−x and FePxN4−x (x=1–4)) on the electronic structure optimization of Fe center and its catalytic performance. Attributing to the optimal Fe 3d orbitals, FePN3 can effectively activate O2 and promote ORR with a low overpotential of 0.29 V, surpassing FeN4 and most reported catalysts. FeSN3 is beneficial to H2O activation and OER, proceeding with an overpotential of 0.68 V, which is superior to FeN4. Both FePN3 and FeSN3 exhibit outstanding thermodynamic and electrochemical stability with negative formation energies and positive dissolution potentials. Hence, the N,P and N,S co‐coordination might provide better catalytic environment than regular N coordination for SACs in ORR and OER. This work demonstrates FePN3/FeSN3 as high‐performance ORR/OER catalysts and highlights N,P and N,S co‐coordination regulation as an effective approach to fine tune high atomically dispersed electrocatalysts.

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Section: Methodsmentioning

confidence: 99%

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Lü

Cao

et al. 2023

ChemSusChem

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“…Among various adsorbent materials, metal-organic frameworks (MOFs) have attracted tremendous attention due to their particular properties, including ultrahigh porosity, controllable pore size, and easy functionalization. [8][9][10] Many approaches have been adopted to improve the CO 2 adsorption and separation performances in MOFs. [11][12][13][14][15] Abid et al investigated the CO 2 adsorption behavior in MIL-96(Al) via second metal Ca coordination, and found that the CO 2 adsorption capacity in MIL-96(Al)-Ca1 was enhanced from 8.09 to 10.22 mmol/g at 273 K and 950 kPa.…”

Section: Introductionmentioning

confidence: 99%

“…One of the key challenges in implementing the CCS strategy is the development of adsorbent materials with excellent CO 2 adsorption and separation performances. Among various adsorbent materials, metal‐organic frameworks (MOFs) have attracted tremendous attention due to their particular properties, including ultrahigh porosity, controllable pore size, and easy functionalization [8–10] . Many approaches have been adopted to improve the CO 2 adsorption and separation performances in MOFs [11–15] .…”

Section: Introductionmentioning

confidence: 99%

Interlayer Expansion in a Layered Metal‐Organic Framework Enhances CO₂Capture and CO₂/N₂Separation

et al. 2022

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Developing efficient CO 2 adsorbent materials and technologies is significant to reduce the increasing greenhouse gases concentration in the atmosphere. Herein, a layered MOF with a porous kagomé lattice (kgm), which owned three phases (kgm-1, kgm-2, and kgm-3) via interlayer expansion, was evaluated as a promising CO 2 capture and separation material by using grand canonical Monte Carlo simulations. Results showed that the interlayer expansion provided additional pore volume, which played a considerable role in CO 2 adsorption and separation. The CO 2 adsorption capacity and CO 2 /N 2 selectivity followed the sequence kgm-3 > kgm-2 > kgm-1, and kgm-3 exhibited an excellent CO 2 adsorption capacity of 8.7 mmol g À 1 at 1 bar with a CO 2 /N 2 selectivity of 130.3 at 20 bar and 298 K. Gas distribution analysis showed that CO 2 and N 2 are adsorbed only in the channels in kgm-1, whereas they could be adsorbed between layers in kgm-2 and kgm-3 due to the interlayer expansion. The adsorption heat and interactions between CO 2 and frameworks were analyzed to elucidate the effect of interlayer expansion. Results of this work highlighted that appropriate interlayer expansion can be an effective approach for framework adsorbents to improve CO 2 capture ability and separation performance at the same time.

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“…Rapidly increasing CO 2 concentration in the atmosphere due to the burning of fossil fuels has resulted in the greenhouse effect. [ 1–4 ] Carbon capture and storage (CCS) has been proposed to alleviate uncontrolled CO 2 emissions. [ 5–7 ] It is essential to develop suitable adsorbent materials to capture CO 2 .…”

Section: Introductionmentioning

confidence: 99%

Functionalized 3D Covalent Organic Frameworks for High‐Performance CO₂ Capture and Separation over N₂

Wei

Xin

Wang

et al. 2022

Advcd Theory and Sims

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Covalent organic frameworks (COFs) are emerging adsorbent materials for CO2 capture and separation due to their tunable pore size, periodic permutation, and chemical thermal stability. Herein, four functionalized 3D COF‐300s (COF‐300‐X, X = –SO3H, –NO2, –OH, and –NH2) for CO2 adsorption and separation are studied by using density functional theory and grand canonical Monte Carlo simulation. The results show that four functionalized COF‐300s could create a feasible environment for CO2 adsorption with high accessible surface area, suitable pore size, and high porosity. The CO2 adsorption capacity in COF‐300s could be significantly improved by functionalization. In comparison, the best performing COF‐300‐SO3H shows a superior CO2 adsorption capacity of 6.23 mmol g−1 and a high CO2/N2 selectivity of 393 at 298 K and 100 kPa. The adsorption heat and interaction analyses demonstrate that the CO2 affinity in COF‐300s is enhanced by the introduction of polar functional groups, which renders great CO2 adsorption and separation performances. The gas distribution shows that the adsorption sites are concentrated near the functional groups and the distribution of CO2 in COF‐300‐SO3H has a characteristic of multilayer adsorptions. This work highlights COF‐300‐SO3H as an outperforming adsorbent candidate for CO2 capture and separation.

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First-row transition metal embedded pyrazine-based graphynes as high-performance single atom catalysts for the CO₂reduction reaction

Abstract: Single atom catalysts (SACs) have displayed unprecedented activity and selectivity toward electrochemical CO2 reduction reaction (CO2RR). Herein, first-row transition metal embedded pyrazine-based graphynes (TM-pyGYs) were evaluated as potential SACs for...

Cited by 30 publications

References 50 publications

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Interlayer Expansion in a Layered Metal‐Organic Framework Enhances CO₂Capture and CO₂/N₂Separation

Functionalized 3D Covalent Organic Frameworks for High‐Performance CO₂ Capture and Separation over N₂

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First-row transition metal embedded pyrazine-based graphynes as high-performance single atom catalysts for the CO2reduction reaction

Abstract: Single atom catalysts (SACs) have displayed unprecedented activity and selectivity toward electrochemical CO2 reduction reaction (CO2RR). Herein, first-row transition metal embedded pyrazine-based graphynes (TM-pyGYs) were evaluated as potential SACs for...

Cited by 30 publications

References 50 publications

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Constructing N,S and N,P Co‐Coordination in Fe Single‐Atom Catalyst for High‐Performance Oxygen Redox Reaction

Interlayer Expansion in a Layered Metal‐Organic Framework Enhances CO2Capture and CO2/N2Separation

Functionalized 3D Covalent Organic Frameworks for High‐Performance CO2 Capture and Separation over N2

Contact Info

Product

Resources

About

First-row transition metal embedded pyrazine-based graphynes as high-performance single atom catalysts for the CO₂reduction reaction

Interlayer Expansion in a Layered Metal‐Organic Framework Enhances CO₂Capture and CO₂/N₂Separation

Functionalized 3D Covalent Organic Frameworks for High‐Performance CO₂ Capture and Separation over N₂