The effect of coordination environment on the activity and selectivity of single-atom catalysts

Zhang, Yuqi; Yang, Jack; Ge, Riyue; Zhang, Jiujun; Cairney, Julie M.; Liu, Ying; Zhu, Mingyuan; Li, Sean; Li, Wenxian

doi:10.1016/j.ccr.2022.214493

Cited by 125 publications

(60 citation statements)

References 250 publications

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“…Future research should focuses on developing precursors with low‐cost, scalability, and versatility features to minimize the requirements of ball milling method. [ 64 ]…”

Section: Synthesis Routes Of Sacsmentioning

confidence: 99%

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

et al. 2022

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Single‐atom catalysts (SACs) attract extensive attention in the field of heterogeneous catalysis in recent years due to the maximum atom utilization and unique physical and chemical properties. The gas sensing is actually a heterogeneous catalysis process but the SACs are new to this area. Although SACs show huge potential in gas sensing, the SACs gas sensing area currently is still at the infancy stage. This work critically reviews the recent advances and current status of single‐atom gas sensing materials. General synthesis routes, characterization methods, and sensing performance indexes are introduced. At the end, the challenges and future prospects on SACs gas sensing are presented from the authors’ perspectives. This work is anticipated to provide insights and guideline for the chemical sensing community.

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“…Future research should focuses on developing precursors with low‐cost, scalability, and versatility features to minimize the requirements of ball milling method. [ 64 ]…”

Section: Synthesis Routes Of Sacsmentioning

confidence: 99%

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

et al. 2022

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“…In the context of peak carbon dioxide emissions and carbon neutrality, highly efficient CO 2 capture and conversion technologies have become increasingly important. − However, due to the high bond energy of the C–O bond, CO 2 molecules are chemically inert and difficult to be activated. , One of the main challenges of the carbon dioxide reduction reaction (CO 2 RR) is to develop catalysts that can break C–O bonds and selectively generate specific products. − Among many CO 2 conversion strategies, electrocatalysis has been widely studied because of its ability to convert CO 2 into high-value-added chemicals and fuels. − …”

Section: Introductionmentioning

confidence: 99%

High-Throughput Computational Screening of Metal–Organic Frameworks as High-Performance Electrocatalysts for CO₂RR

et al. 2022

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Metal–organic frameworks (MOFs) are considered as promising electrocatalytic materials for the carbon dioxide reduction reaction (CO2RR) due to their various excellent properties. Here, through multistep high-throughput screening of the Computation-Ready, Experimental (CoRE) MOF database, including structural rationality check, pore size screening, adsorption capacity prediction, open metal site identification, CO2 molecular activation capacity, and reaction path calculation, MOFs named GAFRUD, CAJQEL, and cg400449c are identified as potential catalysts for electrocatalytic CO2RR. Furthermore, based on density functional theory calculations, we propose that the polarity of the coordination bonds between the metal atoms and the coordination atoms in ligands has a significant impact on the activation of CO2 molecules, and the selectivity of HCOOH mainly depends on the adsorption energy difference between *HCOO and *COOH. This principle is further validated by the experimental results, which will provide guidelines for the rational design of MOF-based electrocatalysts for CO2RR.

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“…A crucial aspect, which is often overlooked or misinterpreted, is that these atoms are defined as “single” because they are not in pairs or in clusters but not because they are “isolated” atoms. , On the contrary, as we said above, they are either supported on a possibly interacting substrate or even embedded in a solid material; thus, they should be actually considered as “coordinated” or “bonded” single atoms. , The relevant consequence of this is that the properties of SACs are not those of an isolated single atom but are those of a single atom embedded in a certain specific surrounding environment, which can be tailored by modifying the chemical nature of the substrate.…”

Section: Introductionmentioning

confidence: 99%

Using Coordination Chemistry Concepts to Unravel Electronic Properties of SACs in Bidimensional Materials

2022

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Single atom catalysts (SACs) embedded in bidimensional (2D) materials are commonly viewed as chemically doped 2D systems whose electronic properties can be discussed in terms of solid state physics, where the doping atoms are perturbating agents to the semimetallic (graphene) or insulating (h-BN) character of the 2D material. In this Perspective, we present a different and closer viewpoint, where the SAC electronic properties are interpreted in terms of coordination chemistry concepts, as the transition metal (TM) atom is complexed by a giant macrocycle, which is the defective 2D layer. In the crystal/ligand field theories, both electrostatic and covalent interactions between SAC and the surrounding 2D material are accounted for defining the splitting and mixing of the TM d states. This analysis reveals the key role played by the type of 2D material not only in determining spin and charge of SAC but also in stabilizing several SAC oxidative states via charge delocalization for an enhanced catalytic activity.

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The effect of coordination environment on the activity and selectivity of single-atom catalysts

Cited by 125 publications

References 250 publications

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

High-Throughput Computational Screening of Metal–Organic Frameworks as High-Performance Electrocatalysts for CO₂RR

Using Coordination Chemistry Concepts to Unravel Electronic Properties of SACs in Bidimensional Materials

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The effect of coordination environment on the activity and selectivity of single-atom catalysts

Cited by 125 publications

References 250 publications

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

Progress and Perspectives of Single‐Atom Catalysts for Gas Sensing

High-Throughput Computational Screening of Metal–Organic Frameworks as High-Performance Electrocatalysts for CO2RR

Using Coordination Chemistry Concepts to Unravel Electronic Properties of SACs in Bidimensional Materials

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Product

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High-Throughput Computational Screening of Metal–Organic Frameworks as High-Performance Electrocatalysts for CO₂RR