Room-Temperature CO Oxidative Coupling for Oxamide Production over Interfacial Au/ZnO Catalysts

Cao, Yanwei; Yao, Peng; Cheng, Danyang; Chen, Lin; Wang, Maolin; Shang, Cheng; Zheng, Lirong; Ma, Ding; Liu, Zhi-Pan; Lin, He

doi:10.1021/acscatal.2c05358

Cited by 14 publications

(9 citation statements)

References 67 publications

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“…Therefore, the coordination of Au at the interface with neighboring O, Zn, and other Au atoms in the cluster or NPs. [ 19 ] This depends on the surface behavior of defective ZnO and the concentration of Au 𝛿+ in photodeposition. The electrons are transferred from Au atom to oxygen vacancies sites to form Au‐O‐Zn linkages at the interface between the Au and ZnO.…”

Section: Resultsmentioning

confidence: 99%

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production

Mohite,

Kim,

Bae

et al. 2023

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Healed defects on photocatalysts surface and their interaction with plasmonic nanoparticles (NPs) have attracted attention in H2 production process. In this study, surface oxygen vacancy (Vo) defects are created on ZnO (Vo‐ZnO) NPs by directly pyrolyzing zeolitic imidazolate framework. The surface defects on Vo‐ZnO provide active sites for the diffusion of single Au atoms and as nucleation sites for the formation of Au NPs by the in situ photodeposition process. The electronically healed surface defects by single Au atoms help in the formation of a heterojunction between the ZnO and plasmonic Au NPs. The formed Au/Vo‐Au:ZnO‐4 heterojunction prolongs photoelectron lifetimes and increases donor charge density. Therefore, the optimized photocatalysts of Au/Vo‐Au:ZnO‐4 has 21.28 times higher H2 production rate than the pristine Vo‐ZnO under UV–visible light in 0.35 m Na2SO4 and 0.25 m Na2SO3. However in 0.35 m Na2S and 0.25 m Na2SO3, the H2 production rate is 25.84 mmole h−1 g−1. Furthermore, Au/Vo‐Au:ZnO‐4 shows visible light activity by generating hot carries via induced surface plasmonic effects. It has 48.58 times higher H2 production rate than pristine Vo‐ZnO. Therefore, this study infers new insight for defect healing mediated preparation of Au/Vo‐Au:ZnO heterojunction for efficient photocatalytic H2 production.

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Section: Resultsmentioning

confidence: 99%

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production

Mohite,

Kim,

Bae

et al. 2023

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“…Overlayers can be used for advanced catalyst fabrication and application , during intense investigation of an SMSI. Particularly, overlayer formation creates a physicochemical partition between the metals, endowing NPs with excellent high-temperature sintering resistance. , In some situations, catalysts with an overlayer exhibit excellent catalytic activity, although the number of metal sites decreases due to encapsulation of the metal surface. − Overlayer structures should be manipulated to understand an SMSI and fabricate high-performance catalysts.…”

Section: Introductionmentioning

confidence: 99%

Atmosphere-Dependent Strong Metal–Support Interactions in Au/ZnO Catalysts and Their Overlayer Permeability

Wu,

Jiang,

Niu

et al. 2024

ACS Catal.

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The oxidative strong metal–support interaction (O-SMSI) emerges as a pioneering approach for promoting the formation of overlayers, which has garnered significant interest in the exploration of the synthesis of O-SMSI materials. However, the manipulation of the overlayer is rarely discussed and presents a challenge due to its trace presence on the nanoparticle (NP) surface, which impedes the development and utilization of the O-SMSI. In this work, we demonstrate a strong correlation between the treatment atmosphere and the state of the permeable overlayer in the Au/ZnO catalyst. The ZnO overlayer can be formed in both oxidative and inert atmospheres, but the permeability of the overlayer occurs under an oxidative atmosphere. The difference in the permeabilities of the overlayer, at similar particle sizes, leads to a reaction rate difference of approximately 1.4 times. While the permeability of the ZnO overlayer is improved by an oxidative atmosphere treatment, it is also accompanied by an increase in the geometric strain in the ZnO matrix. The permeable ZnO formation is related to the process of gold species insertion into the ZnO matrix, as indicated by density functional theory calculations. This study is the first to describe the role of O2 in manipulating the O-SMSI and suboxide overlayers, offering a potential method for surface engineering.

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“…GJena et al revealed the effects of binding single hydrogen atoms in gold clusters through theoretical calculations [ 57 ]; this showed that introducing impurities such as H atoms in gold clusters can be highly efficient and cost-effective compared with using pristine gold clusters for CO oxidation. For example, He et al reported a highly selective Au/ZnO composite catalyst for the one-step oxidative coupling of CO with secondary amines, producing oxamides [ 58 ]. SiAu silicides were experimentally reported in early 1964 by Barrow et al [ 59 ].…”

Section: Introductionmentioning

confidence: 99%

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

Zhang

Ren

2023

Molecules

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Significant progress has been made in understanding the reactivity and catalytic activity of gas-phase and loaded gold clusters for CO oxidation. However, little research has focused on mixed silicon/gold clusters (SiAun) for CO oxidation. In the present work, we performed density function theory (DFT) calculations for a SiAun (n = 1–5) cluster at the CAM-B3LYP/aug-cc-pVDZ-PP level and investigated the effects on the reactivity and catalytic activity of the SiAun cluster for CO oxidation. The calculated results show that the effect is very low for the activation barriers for the formation of OOCO intermediates on SiAu clusters, SiAu3 clusters, and SiAu5 clusters in the catalytic oxidation of CO and the activation energy barriers for the formation of OCO intermediates on OSiAu3, OSiAu4, and OSiAu5. Our calculations show that, compared with the conventional small Au cluster, the incorporation of Si enhances the catalytic performance towards CO oxidation.

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Room-Temperature CO Oxidative Coupling for Oxamide Production over Interfacial Au/ZnO Catalysts

Cited by 14 publications

References 67 publications

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production

Atmosphere-Dependent Strong Metal–Support Interactions in Au/ZnO Catalysts and Their Overlayer Permeability

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

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Room-Temperature CO Oxidative Coupling for Oxamide Production over Interfacial Au/ZnO Catalysts

Cited by 14 publications

References 67 publications

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H2 Production

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H2 Production

Atmosphere-Dependent Strong Metal–Support Interactions in Au/ZnO Catalysts and Their Overlayer Permeability

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

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Product

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Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production

Defects Healing of the ZnO Surface by Filling with Au Atom Catalysts for Efficient Photocatalytic H₂ Production