A Supported Nickel Catalyst Stabilized by a Surface Digging Effect for Efficient Methane Oxidation

Zhou, Huang; Liu, Tianyang; Zhao, Xuyan; Zhao, Yafei; Lv, Hongwei; Fang, Shi; Wang, Xiaoqian; Zhou, Fangyao; Xu, Qian; Xu, Jie; Xiong, Can; Xue, Zhenggang; Wang, Kai; Cheong, Weng‐Chon; Xi, Wei; Gu, Lin; Yao, Takeshi; Wei, Shiqiang; Hong, Xun; Luo, Jun; Li, Yafei; Wu, Yuen

doi:10.1002/anie.201912785

Cited by 84 publications

(49 citation statements)

References 25 publications

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“…[72] Furthermore, by utilizing the strong coordination interaction between the N-rich defects and surface Ni atoms, Wu and co-workers developed a surface digging effect for Ni NPs on amorphous NC, and synthesized a stable sinteringresistant supported Ni SACs on carbon nanotubes. [73] In situ TEM observations and theoretical calculations revealed that the Ni NPs on the surface would be etched and anchored in the NC support. Besides, they developed a N-doped carbon thermal atomization strategy to treat severely deactivated and sintered .…”

Section: Active Sites Of Sacsmentioning

confidence: 99%

General Design Concept for Single‐Atom Catalysts toward Heterogeneous Catalysis

et al. 2021

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state of the catalyst, it can be classified as three types: homogeneous catalyst, heterogeneous catalyst, and biological (enzyme) catalyst. [4,5] Among them, the heterogeneous catalyst is the most important one because of its strong stability under severe conditions (e.g., high temperature, high pressure) and easy recovery from the reactants and products. [6,7] Heterogeneous catalyst is usually in the form of welldispersed metal particles and clusters, each of which may have multiple active sites with different properties. [8] It is well known that the coordination environment and electronic structure of metal-centered sites are the decisive factors in affecting the catalytic performance. However, traditional heterogeneous catalysts usually suffer from the insufficient utilization of atom, because only a small fraction of surface metal atoms can participate in the reaction. To reduce the cost of heterogeneous catalysis and improve the utilization efficiency of active metals in the heterogeneous catalyst, to rationally design and develop catalytic materials with good activity, durability and selectivity is now of greatest concern.Last decades, the gradual development of various precision instruments and detection methods has greatly stimulated the interests in the observation and exploration of microcosms. [9][10][11][12][13][14][15][16][17][18] Therefore, nanocatalysis, a new era of catalytic research, has been introduced and promoted by the rapid development of nanoscience. Studies have shown that the performance of catalyst can be determined by the size of catalytic metal particles. By controlling the nucleation and growth processes at nanoscale, nanoparticles (NPs) with high surface-to-volume ratios can be obtained. [19][20][21][22][23] Moreover, the abundant coordination unsaturated surface atoms located at edges, corners, and steps along with specific morphology of nanoparticles both have an important effect on the adsorption, desorption and activation process of small molecule reactants, which can effectively modulate the catalytic efficiency. [24] To obtain high atomic utilization efficiency, the particle of active metal is continuously reduced from nanoscale to sub-nanometer-scale or even atomic scale. [25,26] To this end, single-atom catalysts (SACs) bring new opportunities to the study in molecularly and atomically catalytic mechanisms, which require the accurate structure design at atomic scale.Compared with NPs catalysts, the metal species of SACs are uniformly dispersed on the support with maximum atom dispersion. [5,7,[27][28][29] Furthermore, the catalytic activities As a new and popular material, single-atom catalysts (SACs) exhibit excellent activity, selectivity, and stability for numerous important reactions, and show great potential in heterogeneous catalysis due to their high atom utilization efficiency and the controllable characteristics of the active sites. The composition and coordination would determine the geometric and electronic structures of SACs, and thus greatly influence the catal...

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Section: Active Sites Of Sacsmentioning

confidence: 99%

General Design Concept for Single‐Atom Catalysts toward Heterogeneous Catalysis

et al. 2021

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“…Methane (CH 4 ) is an important fossil fuel and a starting point of C1 chemistry. Efficient utilization of CH 4 is an imperative task [1–7] . CH 4 is the most thermodynamically stable alkane and has a first bond dissociation energy as high as 439.3 kJ mol −1 [2, 8] .…”

Section: Figurementioning

confidence: 99%

“…Efficient utilization of CH 4 is an imperative task. [1][2][3][4][5][6][7] CH 4 is the most thermodynamically stable alkane and has a first bond dissociation energy as high as 439.3 kJ mol À1 . [2,8] The chemical inertness of CH 4 make its conversion energy-intensive, reflected by industrial production of hydrogen (H 2 ) based on the highly endothermic methane steam reforming (MSR, CH 4 + 2 H 2 OÐCO 2 + 4 H 2 ) at temperatures higher than 700 8C.…”

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confidence: 99%

Electrochemical Splitting of Methane in Molten Salts To Produce Hydrogen

Fan

Xiao

2021

Angewandte Chemie

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Industrial hydrogen production based on methane steam reforming (MSR) remains challenges in intensive carbon emissions, retarded hydrogen generation owing to coke deposition over catalysts and huge consumption of water. We herein report an electrochemical splitting of methane (ESM) in molten salts at 500 8C to produce hydrogen in an energy saving, emission-free and water-free manner. Following the most energy-saving route on methane-to-hydrogen conversion, methane is electrochemically oxidized at anode to generate carbon dioxide and hydrogen. The generated anodic carbon dioxide is in situ captured by the melts and reduced to solid carbon at cathode, enabling a spatial separation of anodic hydrogen generation from cathodic carbon deposition. Lifecycle assessment on hydrogen-generation technologies shows that the ESM experiences an equivalent carbon emission much lower than MSR, and a lower equivalent energy input than alkaline water electrolysis.

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“…Thus, Li et al. combined AC−HAADF−STEM with in situ TEM to observe the formation of Ni SACs from Ni NPs [145] . As shown in Figures 8a‐8c, the transformation from Ni NPs to Ni SACs can be gradually completed in the first 3 h, accompanied with the explosion of surface holes.…”

Section: Characterization Of Sacsmentioning

confidence: 99%

Section: Electron Microscopy With Atomic Resolutionmentioning

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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A Supported Nickel Catalyst Stabilized by a Surface Digging Effect for Efficient Methane Oxidation

Cited by 84 publications

References 25 publications

General Design Concept for Single‐Atom Catalysts toward Heterogeneous Catalysis

General Design Concept for Single‐Atom Catalysts toward Heterogeneous Catalysis

Electrochemical Splitting of Methane in Molten Salts To Produce Hydrogen

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

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