Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions

Cao, Sufeng; Yang, Ming; Elnabawy, Ahmed O.; Trimpalis, Antonios; Li, Sha; Wang, Chongyang; Göltl, Florian; Chen, Zhihengyu; Liu, Jilei; Shan, Junjun; Li, Mengwei; Haas, T. E.; Chapman, Karena W.; Lee, Sungwon; Allard, Lawrence F.; Mavrikakis, Manos; Flytzani‐Stephanopoulos, Maria

doi:10.1038/s41557-019-0345-3

Cited by 92 publications

(52 citation statements)

References 38 publications

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“…[ 5–8 ] Featuring with atomically dispersed and uniformly distributed metal centers, recently, transition metal single‐atomic‐site (SAS) catalysts with MNC structures have drawn intensive research attention and hold great potential to substitute Pt in ORR under alkaline condition. [ 9–23 ] Among them, Fe‐based SAS catalysts exhibit excellent ORR activities; however, their performances after being assembled in metal–air batteries are not satisfactory. [ 21–24 ] It is generally believed that the ORR reaction is limited by the difficulty of *OH desorption from the active sites of SAS catalysts, which is dependent on the nature of the transition metal.…”

Section: Introductionmentioning

confidence: 99%

MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

Han

Zhang

Chen

et al. 2020

Advanced Energy Materials

103

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The development of inexpensive and highly efficient nonprecious metal catalysts to substitute Pt in the alkaline oxygen reduction reaction is an appealing idea in the energy field. Herein, a Mn oxygen reduction electrocatalyst with a half‐wave potential (E1/2) as high as 0.910 V under an alkaline oxygen reduction reaction process is developed, and the dynamic atomic structure change of the highly efficient Mn single‐atomic site is investigated using operando X‐ray absorption spectroscopy. These results demonstrate that the low‐valence MnL+N4 is the active site during the oxygen reduction process. Density functional theory reveals that facile electron transfer from MnL+N4 to adsorbed *OH species plays a key role in the excellent electrocatalytic performance. Moreover, when assembled as the cathode in a zinc–air battery, this MnN4 material shows high power density and excellent durability, demonstrating its promising potential to substitute the Pt catalyst in practical devices.

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Section: Introductionmentioning

confidence: 99%

MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

Han

Zhang

Chen

et al. 2020

Advanced Energy Materials

103

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“…[88][89][90] Atomically dispersed Au and Pt have been reported, demonstrating how they exist in atomic form, and suggesting their potentials for catalytic reactions. [91][92][93][94] For single-atom catalysts, isolating single atoms on the supports and the corresponding catalytic reactions remains challenging.…”

Section: Atomically Doped Plasmonic Metalmentioning

confidence: 99%

Enhancing the Photocatalytic Activity of TiO₂ Catalysts

Jeon

Kweon

Jang

et al. 2020

Advanced Sustainable Systems

102

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charge separation and intrinsic efficiency, which are limited by the material's wide bandgap (≈3 eV). To overcome these issues, countless studies have focused on modifying the properties of TiO 2 , such as controlling its crystal structures, morphologies, vacancies, and doping. Existing natural TiO 2 polymorphs, the anatase and rutile phases, are generally considered representative photocatalytic materials. However, brookite has not been actively studied because in the past it has been difficult to synthesize. Anatase is known to more efficiently separate photoexcited charge carriers than rutile, but its thermodynamic stability has the reverse tendency. [14,15] While studying the different properties of various TiO 2 crystal structures, morphology-dependent characteristics have also been investigated, including efficient charge carrier dynamics, which include longer charge carrier diffusion length than the particle size to separate charges suppressing charge recombination. In addition to these high-crystalline-controlled studies, defect engineering approaches have also been vigorously investigated, to extend the material's light absorption range from the ultraviolet (UV) region to visible light. The general method used to enhance photocatalytic performance has been to introduce defects into TiO 2 structures, by chemical and physical doping, and induce vacancies in titanium (Ti) or oxygen (O) positions. These defect engineering strategies create new energy states, which act as charge trapping sites or narrowing bandgap to extend light absorption region. The formation of new energy states and defect sites is dependent on synthesis methods and conditions, indicating that predicting property and mechanism of synthesized TiO 2 materials is difficult before testing catalytic reactions. This uncertainty is one of the main problems to design new high-performance catalysts. Up to now, numerous researches have been reported to enhance photocatalytic activities and to reveal the mechanism. Even though it has not been confirmed the mechanism and activity for all situations, we can get insight for comprehensive understanding to predict and to design new catalysts. This work reviews modifying strategies of TiO 2 materials to enhance their photocatalytic activity with categorizing in the several systems. First, the basic principles of photocatalytic reactions on TiO 2 are described. Second, the characteristics of surface modification with other elements and doped systems in the lattice of photocatalysts are discussed. Finally, multicomponent heterostructure systems and current photocatalyst To address energy and environmental problems, innumerable titanium dioxide (TiO 2)-based photocatalysts have been reported over the last four decades. TiO 2 has attracted immense interest because it is low-cost, abundant, and photoresponsive. Sunlight-driven fuel production is one of the ideal photocatalytic approaches in terms of economics and the environment. However, performance issues with TiO 2 photocatalysts remain, including insuffici...

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“…Thus, a suitable substrate, which can offer strong metal‐support interactions, is essential for the synthesis of high metal loading SACs. Besides, smart strategies are required to prepare high metal loading SACs [27,94–97] . Usually, atoms like nitrogen (N) [98] and sulfur (S) [99] that contain lone pairs of electrons, have robust coordination ability with metal atoms, serving as coordination sites to stabilize single metal atoms.…”

Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

“…Besides, smart strategies are required to prepare high metal loading SACs. [27,[94][95][96][97] Usually, atoms like nitrogen (N) [98] and sulfur (S) [99] that contain lone pairs of electrons, have robust coordination ability with metal atoms, serving as coordination sites to stabilize single metal atoms. Therefore, constructing coordination atoms, as anchoring sites, is an effective approach to synthesizing high metal loading SACs.…”

Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Wang

Liu

2020

ChemCatChem

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Single‐atom catalysts (SACs) have been rising recently as a new frontier in the catalysis field. Due to maximum atom utilization efficiency and tunable electronic structures, SACs exhibit highly distinctive catalytic performance from bulk counterparts. SACs with high metal loading will facilitate practical applications. To that end, this Review focuses on recent strategies to maximize metal loading. An appropriate substrate, mainly heteroatom‐doped carbon materials, is the key to avoiding aggregation or sintering during synthetic procedures. The coordination site construction and spatial confinement strategies are adopted to prepare SACs with high metal loading. Advanced characterization techniques with atomic resolution are indispensable for identification of the exact structure of SACs. This is true, especially for the applications and challenges in developing in situ/operando characterization techniques at the atomic level, which are discussed in this Review. Moreover, it is fundamentally necessary to investigate the active center structure, which facilitates any design of efficient SACs that can maximize single‐atom catalytic activity. Furthermore, this Review highlights challenges and prospects for development of SACs.

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Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions

Cited by 92 publications

References 38 publications

MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

Enhancing the Photocatalytic Activity of TiO₂ Catalysts

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

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Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions

Cited by 92 publications

References 38 publications

MnN4 Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

MnN4 Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

Enhancing the Photocatalytic Activity of TiO2 Catalysts

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

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Product

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MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

MnN₄ Oxygen Reduction Electrocatalyst: Operando Investigation of Active Sites and High Performance in Zinc–Air Battery

Enhancing the Photocatalytic Activity of TiO₂ Catalysts