Research Progress of Hydrogen Sulfide Adsorption Based on MOFs

Liu, Ying

doi:10.1002/slct.202102950

Cited by 11 publications

(5 citation statements)

References 43 publications

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“…Although H2S adsorption has been studied in a range of MOFs, [47][48][49][50][51][52][53][54][55] the majority of these frameworks are not suitable for therapeutic transdermal delivery. This limitation is a consequence of the presence of toxic or air-sensitive metal centers as well as their relatively weak interaction with H2S, leading to its rapid loss upon exposure to air.…”

Section: Resultsmentioning

confidence: 99%

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Mandel,

Lotlikar,

Runcevski

et al. 2024

Preprint

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Hydrogen sulfide (H2S) is an endogenously produced gasotransmitter involved in many physiological processes that are integral to proper cellular functioning, including chemical signaling, redox balancing, and modification of vital proteins. Due to its profound anti-inflammatory and antioxidant properties, H2S plays important roles in preventing inflammatory skin disorders and improving wound healing. Transdermal H2S delivery is a therapeutically viable option for the man-agement of such disorders. However, current small-molecule H2S donors are not optimally suited for transdermal deliv-ery and typically generate electrophilic byproducts that may lead to undesired toxicity. Here, we demonstrate that H2S release from metal-organic frameworks (MOFs) bearing coordinatively unsaturated metal centers is a promising alterna-tive for controlled transdermal delivery of gaseous H2S without the release of unwanted byproducts. In particular, exten-sive gas sorption measurements and powder X-ray diffraction (PXRD) studies of eleven MOFs support that the Mg-based framework Mg2(dobdc) (dobdc4− = 2,5-dioxidobenzene-1,4-dicarboxylate) is uniquely well-suited for transdermal H2S delivery due to its strong yet completely reversible binding of H2S, high capacity (14.7 mmol/g or 33.3 wt% at 1 bar and 25 °C), and lack of toxicity. In addition, Rietveld refinement of high-quality synchrotron PXRD data from a H2S-dosed mi-crocrystalline sample of Mg2(dobdc) supports that the high H2S capacity of this framework arises due to the presence of three distinct binding sites: at the Mg centers through a Mg⋅⋅⋅S interaction (primary site), through a short S⋅⋅⋅S interaction to the polarized H2S molecules at the primary sites (secondary site), and in the center of the pores (tertiary site). Last, we demonstrate that transdermal delivery of H2S from this framework is sustained over a 24 h period through porcine skin. Not only is this significantly longer than sodium sulfide (Na2S), but this represents the first example of controlled trans-dermal delivery of pure H2S gas. Overall, H2S-loaded Mg2(dobdc) is an easily accessible, solid-state source of H2S, ena-bling safe storage and transdermal delivery of this therapeutically relevant gas.

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Section: Resultsmentioning

confidence: 99%

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Mandel,

Lotlikar,

Runcevski

et al. 2024

Preprint

View full text Add to dashboard Cite

show abstract

“…Although H 2 S adsorption has been studied in a range of MOFs, − mostly in the context of H 2 S removal from contaminated gas streams, the majority of these frameworks are not suitable for therapeutic transdermal delivery. This limitation is a consequence of the presence of toxic or air-sensitive metal centers, such as in the case of MIL-53(Cr) (MIL = Matériaux de l'Institut Lavoisier), as well as their relatively weak interaction with H 2 S, leading to its rapid loss upon exposure to air .…”

Section: Resultsmentioning

confidence: 99%

Transdermal Hydrogen Sulfide Delivery Enabled by Open-Metal-Site Metal–Organic Frameworks

Mandel,

Lotlikar,

Runčevski

et al. 2024

J. Am. Chem. Soc.

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Hydrogen sulfide (H 2 S) is an endogenously produced gasotransmitter involved in many physiological processes that are integral to proper cellular functioning. Due to its profound anti-inflammatory and antioxidant properties, H 2 S plays important roles in preventing inflammatory skin disorders and improving wound healing. Transdermal H 2 S delivery is a therapeutically viable option for the management of such disorders. However, current small-molecule H 2 S donors are not optimally suited for transdermal delivery and typically generate electrophilic byproducts that may lead to undesired toxicity. Here, we demonstrate that H 2 S release from metal−organic frameworks (MOFs) bearing coordinatively unsaturated metal centers is a promising alternative for controlled transdermal delivery of H 2 S. Gas sorption measurements and powder X-ray diffraction (PXRD) studies of 11 MOFs support that the Mg-based framework Mg 2 (dobdc) (dobdc 4− = 2,5-dioxidobenzene-1,4-dicarboxylate) is uniquely well-suited for transdermal H 2 S delivery due to its strong yet reversible binding of H 2 S, high capacity (14.7 mmol/g at 1 bar and 25 °C), and lack of toxicity. In addition, Rietveld refinement of synchrotron PXRD data from H 2 S-dosed Mg 2 (dobdc) supports that the high H 2 S capacity of this framework arises due to the presence of three distinct binding sites. Last, we demonstrate that transdermal delivery of H 2 S from Mg 2 (dobdc) is sustained over a 24 h period through porcine skin. Not only is this significantly longer than sodium sulfide but this represents the first example of controlled transdermal delivery of pure H 2 S gas. Overall, H 2 S-loaded Mg 2 (dobdc) is an easily accessible, solid-state source of H 2 S, enabling safe storage and transdermal delivery of this therapeutically relevant gas.

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“…Hydrogen sulfide, as a strong reducing gas molecule, is notorious for its toxicity for several metal oxide gas sensing materials, leading to deteriorated performance or even permanent damage to the sensing materials. , To lift the influence from H 2 S, high-temperature annealing is commonly adopted. In fact, H 2 S molecules can be easily decomposed onto the surface of metal oxides, causing S coverage or oxygen ion replacement on the metal oxides’ surface. − However, the poisoning effect is inadequately studied, leading to the interferences and inaccuracy during gas detection.…”

Section: Introductionmentioning

confidence: 99%

Response Enhancement in High-Temperature H₂S-Treated Metal Oxide Gas Sensors

Chen,

Liu,

Liu

et al. 2024

ACS Sens.

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Metal oxide gas sensors (MOGS), crucial components in monitoring air quality and detecting hazardous gases, are well known for their poisoning effects when exposed to certain gas molecules, such as hydrogen sulfide. Surprisingly, our research reveals that high-temperature H 2 S treatment leads to an enhancement effect rather than response decay. This study investigates the time-decaying response enhancement, being attributed to the formation of metal sulfide and metal sulfate on the metal oxide's surface, enhancing the electronic sensitization. Such an enhancement effect is demonstrated for various gases, including CO, CH 3 CH 2 OH, CH 4 , HCHO, and NH 3 . Additionally, the impacts of H 2 S treatment on the response and recovery time are also observed. Surface compositional analysis are conducted with X-ray photoelectron spectroscopy. A proposed mechanism for the enhancement effect is elaborated, highlighting the role of electronic sensitization and the sulfide−sulfate component. This research offers valuable insights into the potential applications of metal oxide sensors in sulfide-presented harsh environments in gas sensing, encouraging future exploration of optimized sensor materials, operation temperature, and the development of hydrogen sulfide poisoning-resistant and higher sensitivity MOGS.

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Research Progress of Hydrogen Sulfide Adsorption Based on MOFs

Cited by 11 publications

References 43 publications

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Transdermal Hydrogen Sulfide Delivery Enabled by Open-Metal-Site Metal–Organic Frameworks

Response Enhancement in High-Temperature H₂S-Treated Metal Oxide Gas Sensors

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Research Progress of Hydrogen Sulfide Adsorption Based on MOFs

Cited by 11 publications

References 43 publications

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Transdermal hydrogen sulfide delivery enabled by open metal site metal-organic frameworks

Transdermal Hydrogen Sulfide Delivery Enabled by Open-Metal-Site Metal–Organic Frameworks

Response Enhancement in High-Temperature H2S-Treated Metal Oxide Gas Sensors

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Response Enhancement in High-Temperature H₂S-Treated Metal Oxide Gas Sensors