Dense Ru single-atoms integrated with sulfoacids for cellulose valorization to isosorbide

Yang, Ying; Ding, Zhongzhen; Ren, Dongcheng; Shang, Cui; Li, Chen W.; Yang, Feng; Zhou, Biao; Hao, Shijie; Sun, Keju; Lee, Sungwon

doi:10.1016/j.mtsust.2023.100494

Cited by 4 publications

(5 citation statements)

References 50 publications

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“…24 Figure 2d illustrates the peak energies of 485.44 and 463.13 eV in the Ru SA/GFs spectrum, which are ascribed to the metallic Ru 3p 1/2 and Ru 3p 3/2 , respectively. 32,37 Notably, the binding energy of the Ru 3p peak of Ru SA/GFs exhibits a positive energy displacement compared to that of Ru NP/GFs (Figure 2d), implying a charge density change within the Ru atom. 32,38 To acquire a better understanding of the coordination environment and electronic state of the Ru atoms within Ru SA/GFs, X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra were employed to probe the Ru K-edge.…”

Section: Resultsmentioning

confidence: 99%

“…This alteration suggests that the Ru species anchored on the GFs through chemical bonding. , Furthermore, the signal of Na in GFs is relatively strong, whereas the Na signal decreases after the deposition of Ru (Figure S3), suggesting that the Na element probably indeed exerts a pronounced influence on the formation of the Ru single atom Figure d illustrates the peak energies of 485.44 and 463.13 eV in the Ru SA/GFs spectrum, which are ascribed to the metallic Ru 3p 1/2 and Ru 3p 3/2 , respectively. , Notably, the binding energy of the Ru 3p peak of Ru SA/GFs exhibits a positive energy displacement compared to that of Ru NP/GFs (Figure d), implying a charge density change within the Ru atom. , …”

Section: Results and Discussionmentioning

confidence: 99%

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Single-Atom Ru Biomimetic Nanozyme for the Electrochemical Sensing of Hydrogen Peroxide

Jia,

Yu,

Hamed

et al. 2024

ACS Appl. Nano Mater.

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A rational design of high-efficiency single atoms represents a desirable goal for the construction of efficient electrochemical devices. Nevertheless, their activity is constricted by the exposure of single atoms to reactants. Herein, novel ruthenium (Ru) single atom anchored on graphene frameworks (GFs) that feature interconnected porous structures (defined as Ru SA/GFs) is synthesized through a one-step photoreduction strategy. Ru SA/GFs possess additional structural merits that favor promoting reactant transport and maximizing the efficacy of single atoms, which manifest notable amplified electrocatalytic-reduction activity toward hydrogen peroxide (H2O2) than that of Ru nanoparticles/GFs, indicating the remarkable biomimetic nanozyme-like activity of Ru SA/GFs toward H2O2. Density functional theory (DFT) calculations reveal that Ru SA/GFs with atomically dispersed Ru significantly facilitate the electrochemical reduction efficiency toward H2O2. In addition, a sensitive Ru SA/GFs-based electrochemical sensing platform for the detection of H2O2 with a low detection limit of 0.063 μM is developed and demonstrated. This work not only exploits an innovative approach to synthesize single-atom Ru anchored on GFs for the construction of an efficient biomimetic H2O2 electrochemical sensor but also contributes to the broader utilization of Ru single atom in the advancement of diverse high-performance electrochemical devices.

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Section: Resultsmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Single-Atom Ru Biomimetic Nanozyme for the Electrochemical Sensing of Hydrogen Peroxide

Jia,

Yu,

Hamed

et al. 2024

ACS Appl. Nano Mater.

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“…The synthesis of isosorbide from sorbitol or even cellulose, however, remains as a technical challenge, because there are a large number of competing reactions that require precise control for obtaining product selectivity and avoiding side reactions such as degradation or polymerization. 266,271 In the future, catalytic dehydration of sorbitol by solid acids in molten or solvent states is likely to have many opportunities. For example, fluidized beds have made it possible for industry to develop continuous processes for converting cellulose into sorbitol and into isosorbide.…”

Section: Sorbitol Applicationsmentioning

confidence: 99%

Chemocatalytic production of sorbitol from cellulose via sustainable chemistry – a tutorial review

Zhou,

Smith,

2024

Green Chem.

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“…Ru 1 / HMCS−SO 3 H SAC with metal−acid bifunctional sites exhibited good reactivity for cellulose hydrogenation to isosorbide. 142 The acidic site of Ru 1 /HMCS−SO 3 H facilitated cellulose hydrolysis to glucose and the dehydration of sorbitol to isosorbate, while Ru SAs promoted glucose hydrogenation to SOR. The hollow structure of the catalyst notably shortened the reaction path and improved the synergism of Ru SAs and acid sites.…”

Section: Acid Conversions 331 Hydrogenation Of Levulinic Acid (La) To...mentioning

confidence: 99%

“…Characterization and computational modeling showed that (Ni–N 4 )···N was the active site, where apparently distorted octahedral coordination and pyridinic N constituted a frustrated Lewis pair for the heterolytic dissociation of H 2 . Ru 1 /HMCS–SO 3 H SAC with metal–acid bifunctional sites exhibited good reactivity for cellulose hydrogenation to isosorbide . The acidic site of Ru 1 /HMCS–SO 3 H facilitated cellulose hydrolysis to glucose and the dehydration of sorbitol to isosorbate, while Ru SAs promoted glucose hydrogenation to SOR.…”

Section: Application Of Sacs In Biomass Chemical Conversionmentioning

confidence: 99%

Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

Chen,

Xiao,

Guo

et al. 2024

ACS Catal.

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Among all renewable energy sources (e.g., solar energy, wind, and biomass), biomass is the only organic carbon resource which has great potential to partly replace nonrenewable fossil resources to produce high value-added chemicals and biofuels. Singleatom catalysts (SACs) have shown compelling prospects and arguably become one of the most active research fields in biomass chemical catalysis due to their fascinating strengths in maximum atomic utilization, highly efficient catalytic reactivity, high selectivity, and good stability. Numerous achievements about the SACs have recently been amassed, including advanced synthesis methods, characterization techniques, and theoretical calculation, allowing us to forecast their working mechanisms and the catalytic roles of metals and coordination sites in the catalytic process. Based on the relevant literatures on SACs over the past few years, this review summarizes the preparation methods of SACs and their catalysis applications for biomass conversions with a special focus on the structure−activity relationship and catalytic reaction mechanism as well as prospects for the future developments of SACs. This review provides fundamental information for the development of the SACs in biomass valorization, clearly stimulating the development in this emerging research field.

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Dense Ru single-atoms integrated with sulfoacids for cellulose valorization to isosorbide

Cited by 4 publications

References 50 publications

Single-Atom Ru Biomimetic Nanozyme for the Electrochemical Sensing of Hydrogen Peroxide

Single-Atom Ru Biomimetic Nanozyme for the Electrochemical Sensing of Hydrogen Peroxide

Chemocatalytic production of sorbitol from cellulose via sustainable chemistry – a tutorial review

Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

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