Auxiliary Ligand‐Coordinated Nanoconfined Hydrophobic Microenvironments in Nickel(II)–Acetylide Framework for Enhanced CO2 Photoreduction Article Swipe
Yingying Qin
,
Jian Lu
,
Chen Zhang
,
Linli Xu
,
Wai‐Yeung Wong
·
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1002/ange.202505883
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1002/ange.202505883
Metal–acetylide frameworks (MAFs), featuring metal‐bis(acetylide) linkages (─C≡C─M─C≡C─), are emerging as a new class of 2D nanomaterials with promise in catalysis. Here, we report a new 2D Ni II –acetylide framework, TPA‐Ni(PR 3 ) 2 ‐GYs, that incorporates the Ni II (PR 3 ) 2 moiety [R = CH 3 (Me), CH 2 CH 3 (Et), and CH 2 CH 2 CH 2 CH 3 (Bu)] into tris(4‐ethynylphenyl)amine‐based graphdiyne framework (TPA‐GDY). As a result, TPA‐Ni(PBu 3 ) 2 ‐GY exhibits an exceptional photocatalytic CO 2 reduction activity of 3807 µmol g −1 h −1 and a high selectivity of 99.4% for CO production upon visible light irradiation. Mechanistic investigations reveal a strong orbital matching effect between the d orbitals of Ni II and the p orbitals of the alkynyl C atoms in organic ligands, which not only accelerates the transfer and separation of photogenerated charge carriers but also reduces the reaction potential barrier for the formation of *COOH intermediates. Furthermore, the high hydrophobicity of the auxiliary coordinated ligands (trialkylphosphines) to Ni center, particularly tributylphosphine, creates a nanoconfined space that enhances both the accessibility of CO 2 and the utilization of Ni II catalytic active sites while inhibiting hydrogen evolution. This study highlights the benefit of modulating the microenvironment around the coordinated metal center to enhance the performance of catalysts with direct metal–acetylide bonding.
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- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1002/ange.202505883
- https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/ange.202505883
- OA Status
- bronze
- References
- 73
- Related Works
- 10
- OpenAlex ID
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Raw OpenAlex JSON
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https://openalex.org/W4408569563Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1002/ange.202505883Digital Object Identifier
- Title
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Auxiliary Ligand‐Coordinated Nanoconfined Hydrophobic Microenvironments in Nickel(II)–Acetylide Framework for Enhanced CO2 PhotoreductionWork title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2025Year of publication
- Publication date
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2025-03-18Full publication date if available
- Authors
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Yingying Qin, Jian Lu, Chen Zhang, Linli Xu, Wai‐Yeung WongList of authors in order
- Landing page
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https://doi.org/10.1002/ange.202505883Publisher landing page
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https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/ange.202505883Direct link to full text PDF
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YesWhether a free full text is available
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bronzeOpen access status per OpenAlex
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https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/ange.202505883Direct OA link when available
- Concepts
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Acetylide, Nickel, Chemistry, Ligand (biochemistry), Chemical engineering, Photochemistry, Nanotechnology, Materials science, Organic chemistry, Receptor, Biochemistry, EngineeringTop concepts (fields/topics) attached by OpenAlex
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0Total citation count in OpenAlex
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73Number of works referenced by this work
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10Other works algorithmically related by OpenAlex
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| referenced_works | https://openalex.org/W4307968328, https://openalex.org/W4294945945, https://openalex.org/W4386047613, https://openalex.org/W4313487997, https://openalex.org/W4361029787, https://openalex.org/W4382050412, https://openalex.org/W4316022104, https://openalex.org/W4220674625, https://openalex.org/W2886763317, https://openalex.org/W2486685044, https://openalex.org/W3132796685, https://openalex.org/W4292513345, https://openalex.org/W4213192107, https://openalex.org/W4403129176, https://openalex.org/W4210402954, https://openalex.org/W4319332768, https://openalex.org/W4391251650, https://openalex.org/W4391931974, https://openalex.org/W4394933470, https://openalex.org/W2884070004, https://openalex.org/W4362607708, https://openalex.org/W4392850454, https://openalex.org/W4385741058, https://openalex.org/W4399495501, https://openalex.org/W3201057958, https://openalex.org/W2054984148, https://openalex.org/W4312091544, https://openalex.org/W4295128439, https://openalex.org/W4401855780, https://openalex.org/W4391032737, https://openalex.org/W2908934650, https://openalex.org/W3041352360, https://openalex.org/W2939043290, https://openalex.org/W3199140204, https://openalex.org/W3214623477, https://openalex.org/W3180288112, https://openalex.org/W4389037392, https://openalex.org/W3084420553, https://openalex.org/W4281571072, https://openalex.org/W4322625366, https://openalex.org/W3036059291, https://openalex.org/W3036413810, https://openalex.org/W2981706444, https://openalex.org/W4386255373, https://openalex.org/W4294783296, https://openalex.org/W4323294451, https://openalex.org/W4307841917, https://openalex.org/W3085214668, https://openalex.org/W4367394314, https://openalex.org/W4382679222, https://openalex.org/W4313424473, https://openalex.org/W1997952206, https://openalex.org/W2066758334, https://openalex.org/W2014166972, https://openalex.org/W2053030648, https://openalex.org/W2000770615, https://openalex.org/W1981368803, https://openalex.org/W2092157292, https://openalex.org/W2012986644, https://openalex.org/W4210370823, https://openalex.org/W4401916766, https://openalex.org/W1810694562, https://openalex.org/W1031578623, https://openalex.org/W1988375149, https://openalex.org/W2132525235, https://openalex.org/W1979544533, https://openalex.org/W4403294669, https://openalex.org/W4404105415, https://openalex.org/W4223455719, https://openalex.org/W4226400058, https://openalex.org/W4399433645, https://openalex.org/W4401397987, https://openalex.org/W4324380542 |
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