Dual‐Metal Interbonding as the Chemical Facilitator for Single‐Atom Dispersions

Zhou, Yao; Song, Erhong; Chen, Wei; Segre, Carlo U.; Zhou, Jiadong; Lin, Yung‐Chang; Zhu, Chao; Ma, Ruguang; Liu, Pan; Chu, Shufen; Thomas, Tiju; Yang, Minghui; Liu, Qian; Suenaga, Kazu; Liu, Zheng; Liu, Jianjun; Wang, Jiacheng

doi:10.1002/adma.202003484

Cited by 129 publications

(98 citation statements)

References 57 publications

(64 reference statements)

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“…[22][23][24][25][26] Till now, many researches of SACs have been focused on the HER. [27][28][29][30][31][32][33] However, there is still some barrier on the way to apply the SACs in the practical hydrogen production. [34,35] To realize the practical use of the single atomic site catalysts, several problems are needed to be considered, such as regulating the catalytic efficiency of metallic center, regulating the conductivity of basement and so on.…”

mentioning

confidence: 99%

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

Yang,

Li,

Tan

et al. 2021

Angew Chem Int Ed

216

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It is still of great difficulty to develop the non‐platinum catalyst with high catalytic efficiency towards hydrogen evolution reaction via the strategies till now. Therefore, it is necessary to develop the new methods of catalyst designing. Here, we put forward the catalyst designed by the electronic metal–support interaction (EMSI), which is demonstrated to be a reliable strategy to find out the high‐efficiency catalyst. We carried out the density functional theory calculation first to design the proper EMSI of the catalyst. We applied the model of M1‐M2‐X (X=C, N, O) during the calculation. Among the catalysts we chose, the EMSI of Rh1TiC, with the active sites of Rh1‐Ti2C2, is found to be the most proper one for HER. The electrochemical experiment further demonstrated the feasibility of the EMSI strategy. The single atomic site catalyst of Rh1‐TiC exhibits higher catalytic efficiency than that of state‐of‐art Pt/C. It achieves a small overpotential of 22 mV and 86 mV at the at the current density of 10 mA cm−2 and 100 mA cm−2 in acid media, with a Tafel slope of 25 mV dec−1 and a mass activity of 54403.9 mA cm−2 mgRh−1 (vs. 192.2 mA cm−2 mgPt−1 of Pt/C). Besides, it also shows appealing advantage in energy saving compared with Pt/C (≈20 % electricity consuming decrease at 2 kA m−2) Therefore, we believe that the strategy of regulating EMSI can act as a possible way for achieving the high catalytic efficiency on the next step of SACs.

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confidence: 99%

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

Yang,

Li,

Tan

et al. 2021

Angew Chem Int Ed

216

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“…Our results have explained the difficulties of the continuous anchoring method to synthesis the DAC as previous works. [ 11b,12c,16 ] Meanwhile, based on our results, we are able to screen out the promising combinations to achieve the stable DAC. The strong energetic contrast between the stabilization and anchoring energies indicate that the simultaneous anchoring of two different metal atoms is the optimal synthesis method.…”

Section: Resultsmentioning

confidence: 99%

Self‐Validated Machine Learning Study of Graphdiyne‐Based Dual Atomic Catalyst

Sun

Dougherty

et al. 2021

Advanced Energy Materials

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Although the atomic catalyst has attracted intensive attention in the past few years, the current progress of this field is still limited to a single atomic catalyst (SAC). With very few successful cases of dual atomic catalysts (DACs), the most challenging part of experimental synthesis still lies in two main directions: the thermodynamic stability of the synthesis and the optimal combination of metals. To address such challenges, comprehensive theoretical investigations on graphdiyne (GDY)‐based DAC are proposed by considering both, the formation stability and the d‐band center modifications. Unexpectedly, it is proven that the introduction of selected lanthanide metals to the transition metals contributes to the optimized stability and electroactivity. With further verification by machine learning, the potential f–d orbital coupling is unraveled as the pivotal factor in modulating the d‐band center with enhanced stability by less orbital repulsive forces. These findings supply the delicate explanations of the atomic interactions and screen out the most promising DAC to surpass the limitations of conventional trial and error synthesis. This work has supplied an insightful understanding of DAC, which opens up a brand new direction to advance the research in atomic catalysts for broad applications.

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Section: Wet-chemical Methodsmentioning

confidence: 99%

Emerging Single‐Atom Catalysts/Nanozymes for Catalytic Biomedical Applications

Wang

2021

Adv Healthcare Materials

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Single-atom catalysts (SACs) are a type of atomically dispersed nanozymes with the highest atom utilization, which employ low-coordinated single atoms as the catalytically active sites. SACs not only inherit the merits of traditional nanozymes, but also hold high catalytic activity and superb catalytic selectivity, which ensure their tremendous application potential in environmental remediation, energy storage and conversion, chemical industry, nanomedicine, etc. Nevertheless, undesired aggregation effect of single atoms during preactivation and reaction processes is significantly enhanced owing to the high surface free energy of single atoms. In this case, appropriate substrates are requisite to prevent the aggregation event through the powerful interactions between the single atoms and the substrates, thereby stabilizing the high catalytic activity of the catalysts. In this review, the synthetic methods and characterization approaches of SACs are first described. Then the application cases of SACs in nanomedicine are summarized. Finally, the current challenges and future opportunities of the SACs in nanomedicine are outlined. It is hoped that this review may have implications for furthering the development of new SACs with improved biophysicochemical properties and broadened biomedical applications.

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Dual‐Metal Interbonding as the Chemical Facilitator for Single‐Atom Dispersions

Cited by 129 publications

References 57 publications

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

Self‐Validated Machine Learning Study of Graphdiyne‐Based Dual Atomic Catalyst

Emerging Single‐Atom Catalysts/Nanozymes for Catalytic Biomedical Applications

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