Tailored D-π Conjugation Boosts Piezocatalytic CO Reduction in a Platinum(II)-Acetylide Framework.
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| Main Authors: | , , , , , , |
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| Format: | Artículo científico |
| Language: | en |
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Advanced science (Weinheim, Baden-Wurttemberg, Germany)
2026
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| _version_ | 1868266041765789697 |
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| author | Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli |
| author_facet | Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli |
| collection | PubMed - marine biology |
| contents | Tailored D-π Conjugation Boosts Piezocatalytic CO Reduction in a Platinum(II)-Acetylide Framework. Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli Piezocatalytic CO reduction offers a sustainable route for converting mechanical energy into chemical fuels. However, its practical implementation demands catalysts that concurrently exhibit a strong piezoelectric response and high catalytic activity. Herein, we report a one-pot synthesis of well-defined metal-acetylide frameworks (TTED-M-AFs; M = Pt, Pd, Ni) incorporating M(PEt) units into an extended graphdiyne-type scaffold via robust ─C≡C─M(PEt)─C≡C─ linkages. These molecular metal-bis(acetylide) motifs function as intrinsic active sites for CO reduction. Under mechanical agitation, the Pt-based framework achieves a CO production rate of 72.03 µmol g h with 92.4% selectivity, outperforming its Pd and Ni analogues by factors of 1.17 and 1.73, respectively-a trend consistent with their piezoelectric coefficients (d = 35, 21.9, and 12.5 pm V). Combined experimental and theoretical analyses reveal that the piezoelectric field in TTED-Pt-AF enhances CO adsorption and promotes local electron accumulation, thereby lowering the activation energy barrier. Furthermore, in situ high-pressure FT-IR spectroscopy demonstrates that the Pt-bis(acetylide) centers exhibit superior electronic synergy with the tetraphenylene-derived π-conjugated matrix under mechanical stress, inducing pronounced d-π orbital hybridization. The exceptional piezocatalytic performance, coupled with a scalable synthesis, underscores the promise of metal-acetylide frameworks as efficient platforms for mechano-driven CO valorization. |
| format | Artículo científico |
| id | pubmed_42206454 |
| institution | PubMed |
| language | en |
| publishDate | 2026 |
| publisher | Advanced science (Weinheim, Baden-Wurttemberg, Germany) |
| record_format | pubmed |
| spellingShingle | Tailored D-π Conjugation Boosts Piezocatalytic CO Reduction in a Platinum(II)-Acetylide Framework. Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli Tailored D-π Conjugation Boosts Piezocatalytic CO Reduction in a Platinum(II)-Acetylide Framework. Zhu, Mude Zhou, Yingtang Wang, Kai Fan, Xiaoyun Ding, Yang Wong, Wai-Yeung Xu, Linli Piezocatalytic CO reduction offers a sustainable route for converting mechanical energy into chemical fuels. However, its practical implementation demands catalysts that concurrently exhibit a strong piezoelectric response and high catalytic activity. Herein, we report a one-pot synthesis of well-defined metal-acetylide frameworks (TTED-M-AFs; M = Pt, Pd, Ni) incorporating M(PEt) units into an extended graphdiyne-type scaffold via robust ─C≡C─M(PEt)─C≡C─ linkages. These molecular metal-bis(acetylide) motifs function as intrinsic active sites for CO reduction. Under mechanical agitation, the Pt-based framework achieves a CO production rate of 72.03 µmol g h with 92.4% selectivity, outperforming its Pd and Ni analogues by factors of 1.17 and 1.73, respectively-a trend consistent with their piezoelectric coefficients (d = 35, 21.9, and 12.5 pm V). Combined experimental and theoretical analyses reveal that the piezoelectric field in TTED-Pt-AF enhances CO adsorption and promotes local electron accumulation, thereby lowering the activation energy barrier. Furthermore, in situ high-pressure FT-IR spectroscopy demonstrates that the Pt-bis(acetylide) centers exhibit superior electronic synergy with the tetraphenylene-derived π-conjugated matrix under mechanical stress, inducing pronounced d-π orbital hybridization. The exceptional piezocatalytic performance, coupled with a scalable synthesis, underscores the promise of metal-acetylide frameworks as efficient platforms for mechano-driven CO valorization. |
| title | Tailored D-π Conjugation Boosts Piezocatalytic CO Reduction in a Platinum(II)-Acetylide Framework. |
| url | https://pubmed.ncbi.nlm.nih.gov/42206454/ |