Water-induced gaseous formaldehyde decomposition using ruthenium organic crystalline particles

Shen, Yangbin; Xu, Ying; Zhang, Ting; Zhan, Yueping; Guo, Chunxian

doi:10.1039/d2cy01636b

Cited by 4 publications

(12 citation statements)

References 46 publications

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“…Additionally, X-ray diffraction (XRD) also confirmed that Ru-TMPD has a highly ordered crystalline structure. The XRD patterns show obvious peaks at 7.2°, 10.1°, 11.7°, 14.3°, 16.7°, 22.7°, and 28.1° . Other Ru-MOFs exhibited in Scheme have similar XRD peaks at 10.1° (Figures S17–S22).…”

Section: Results and Discussionmentioning

confidence: 88%

“…The XRD patterns show obvious peaks at 7.2°, 10.1°, 11.7°, 14.3°, 16.7°, 22.7°, and 28.1°. 33 Other Ru-MOFs exhibited in Scheme 2 have similar XRD peaks at 10.1°(Figures S17−S22 Ru-TMPD has a high catalytic activity for hydrogen production from acetaldehyde and water reforming. As exhibited in Figure 2a, the gas is produced continuously in a 6 M acetaldehyde solution at 60 °C after Ru-TMPD is added to the solution.…”

Section: ■ Results and Discussionmentioning

confidence: 92%

“…All of the MOFs in Scheme 2 have small specific surface areas. 33 As exhibited in Table 1, the specific surface areas of the MOFs are from 5.71 to 22.50 m 2 g −1 . There is no obvious regularity between the specific surface area and the MOFs, but the average pore radius increases with the ligand length of the MOFs.…”

Section: ■ Results and Discussionmentioning

confidence: 93%

“…The binding energy of N 1s is 399.2 eV in Ru-TMPD, which could be assigned to aromatic ring-connected NH 2 . 33 The coordination effect in Ru-TMPD causes a redshift in the NH 2 Fourier transform infrared (FTIR) absorption spectra (Figure S10).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The yellow suspension was filtered by a filter membrane and washed with hot ethanol. Last, we obtained Ru-TMPD after the yellow powder was dried under vacuum . The other six kinds of Ru-MOFs were prepared by a similar process.…”

Section: Methodsmentioning

confidence: 99%

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Ruthenium Metal–Organic Frameworks as Stable Nanostructures for Selective Hydrogen Production from Acetaldehyde and Water under Mild Conditions

Shen

Zhang

et al. 2023

ACS Appl. Nano Mater.

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Hydrogen is a promising energy carrier because it is a wide and sustainable source. However, it is still extremely difficult to store and transport hydrogen safely because of its active chemical properties and harsh explosion limits. Organic liquid is a popular research field for hydrogen production and storage. Inspired by its biological metabolism, here acetaldehyde is innovatively used for hydrogen production. The hydrogen content of an acetaldehyde–water solution is 10.2 wt %, which is slightly lower than that of a methanol–water solution but much higher than that of formic acid and formaldehyde. For the first time, we prepared several ruthenium metal–organic frameworks (MOFs) as stable nanostructures for selective hydrogen production from acetaldehyde and water under mild conditions (∼60 °C). Ru-MOFs all have nanoscale pores, and the turnover frequency of ruthenium 2,3,5,6-tetramethyl-1,4-phenylenediamine for acetaldehyde decomposition is up to 223 h–1 in water at 90 °C. Because C–C bond cleavage is an inevitable step for hydrogen or energy production from C2 organics, ion chromatography, high-performance liquid chromatography, 1H NMR spectroscopy, and mass spectrometry were employed to propose a catalytic process of hydrogen production from acetaldehyde decomposition. We evidently prove that water participates in acetaldehyde decomposition, thereby claiming an acetaldehyde–water reforming process. Additionally, we confirm that formic acid and acetic acid are the intermediates during the hydrogen production process. This research not only holds great promise for hydrogen production from C2 organics at low temperatures, as well as catalytic technology for C–C bond cleavage, but it also provides certain profound scientific insights for hydrogen or energy production from multicarbon organics, such as biomass.

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Section: Results and Discussionmentioning

confidence: 88%

Section: ■ Results and Discussionmentioning

confidence: 92%

Section: ■ Results and Discussionmentioning

confidence: 93%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 3 more Smart Citations

Ruthenium Metal–Organic Frameworks as Stable Nanostructures for Selective Hydrogen Production from Acetaldehyde and Water under Mild Conditions

Shen

Zhang

et al. 2023

ACS Appl. Nano Mater.

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Hydrogen Production through Distinctive C−C Cleavage during Acetic Acid Reforming at Low Temperature

Shen,

Yang,

Tang

et al. 2024

ChemSusChem

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Acetic acid reforming is a green method for sustainable hydrogen production owing to its renewable source from biomass conversion. However, conventional acetic acid reforming would produce various byproducts, including CO, CH4 and so on. Here, we develop a distinctive method for selective hydrogen production from C‐C directional cleavage during acetic acid reforming. Completely different from conventional acetic acid reforming process, acetic acid would react with water over organoruthenium catalyst during its C‐C cleavage at low temperature, then produce methanol and formic acid (CH3COOH+H2O→CH3OH+HCOOH). Lastly, methanol and formic acid could further decompose into hydrogen and carbon dioxide over organoruthenium selectively.Hydrogen production rate is up to 26.8 molH2/(h‐1*mol‐1Ru) at 150 ℃ through a tandem catalysis. A mechanism for C‐C cleavage of acetic acid is proposed based on intermediate product analysis and density functional theory (DFT) calculation. Firstly, the C‐C single bond was transformed into C=C double bond by dropping one H atom to organoruthenium. Then the coming H2O molecule reacted with the C=C bond by an addition reaction, forming methanol and formic acid. This research not only proposes distinctive reaction pathway for hydrogen production from acetic acid reforming, but also provides some inspiration for selective C‐C bond cleavage during ethanol reforming.

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Catalytic Hydrogen Production from Formaldehyde over Immobilized Ruthenium Complexes

Zhan

Zhou

et al. 2023

Catal Lett

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Water-induced gaseous formaldehyde decomposition using ruthenium organic crystalline particles

Abstract: Formaldehyde is a hydrogen-containing chemical, it could react with water, making formaldehyde-water emerge as an attractive hydrogen storage system. However, formaldehyde also causes carcinogenic airborne pollutants released from paint, coating...

Cited by 4 publications

References 46 publications

Ruthenium Metal–Organic Frameworks as Stable Nanostructures for Selective Hydrogen Production from Acetaldehyde and Water under Mild Conditions

Ruthenium Metal–Organic Frameworks as Stable Nanostructures for Selective Hydrogen Production from Acetaldehyde and Water under Mild Conditions

Hydrogen Production through Distinctive C−C Cleavage during Acetic Acid Reforming at Low Temperature

Catalytic Hydrogen Production from Formaldehyde over Immobilized Ruthenium Complexes

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