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1.
Angew Chem Int Ed Engl ; 61(51): e202212164, 2022 12 19.
Artigo em Inglês | MEDLINE | ID: mdl-36240785

RESUMO

The production of conjugated C4-C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)-atomically doped mesoporous silica, denoted as AlNb-MCM-41, which affords quantitative conversion of 2-methyltetrahydrofuran (2-MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of AlIII and NbV sites into the framework of AlNb-MCM-41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X-ray absorption, diffuse reflectance infrared and solid-state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2-MTHF over AlNb-MCM-41. Specifically, the atomically-dispersed NbV sites play an important role in binding 2-MTHF to drive the conversion. Overall, this study highlights the potential of hetero-atomic mesoporous solids for the manufacture of renewable materials.


Assuntos
Alcadienos , Nióbio , Nióbio/química , Alumínio , Catálise
2.
Angew Chem Weinheim Bergstr Ger ; 134(51): e202212164, 2022 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-38505214

RESUMO

The production of conjugated C4-C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)-atomically doped mesoporous silica, denoted as AlNb-MCM-41, which affords quantitative conversion of 2-methyltetrahydrofuran (2-MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of AlIII and NbV sites into the framework of AlNb-MCM-41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X-ray absorption, diffuse reflectance infrared and solid-state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2-MTHF over AlNb-MCM-41. Specifically, the atomically-dispersed NbV sites play an important role in binding 2-MTHF to drive the conversion. Overall, this study highlights the potential of hetero-atomic mesoporous solids for the manufacture of renewable materials.

3.
World Dev ; 139: 105311, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33250552

RESUMO

The COVID-19 pandemic and ensuing socioeconomic impact on already marginalised refugee communities demonstrate both the need for, and lack of, localisation in humanitarian and development responses. Our research with organisations founded and led by refugees, termed here refugee-led organisations (RLOs), in camps and cities in Kenya and Uganda shows their potential to be an asset in the response to COVID-19 and in contributing to more effective and participatory forms of humanitarian assistance. In this research note we draw on pre-pandemic research with around 80 RLOs and follow-up research with 15 in Uganda and Kenya who are actively responding to the pandemic and its effects. We identify five key areas in which refugees are or could be involved as responders to COVID-19 and other pandemics: providing public information, supplementing capacity gaps, healthcare delivery, shaping social norms, and virus tracking and contact tracing. Our research during COVID-19 shows how RLOs have pivoted their existing service provision to fill assistance gaps, including in areas directly related to public health. As the humanitarian system searches for ways to implement remote and participatory approaches to refugee assistance, RLOs offer great potential, if mechanisms can be found to identify those that are effective, provide them with funding, and build their capacities.

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