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- Cai, Liangliang, et al.
(author)
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Direct Formation of C-C Double-Bonded Structural Motifs by On-Surface Dehalogenative Homocoupling of gem-Dibromomethyl Molecules
- 2018
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In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 12:8, s. 7959-7966
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Journal article (peer-reviewed)abstract
- Conductive polymers are of great importance in a variety of chemistry-related disciplines and applications. The recently developed bottom-up on-surface synthesis strategy provides us with opportunities for the fabrication of various nanostructures in a flexible and facile manner, which could be investigated by high-resolution microscopic techniques in real space. Herein, we designed and synthesized molecular precursors functionalized with benzal gem-dibromomethyl groups. A combination of scanning tunneling microscopy, noncontact atomic force microscopy, high-resolution synchrotron radiation photoemission spectroscopy, and density functional theory calculations demonstrated that it is feasible to achieve the direct formation of C-C double-bonded structural motifs via on-surface dehalogenative homocoupling reactions on the Au(111) surface. Correspondingly, we convert the sp(3)-hybridized state to an sp(2)-hybridized state of carbon atoms, i.e., from an alkyl group to an alkenyl one. Moreover, by such a bottom-up strategy, we have successfully fabricated poly(phenylenevinylene) chains on the surface, which is anticipated to inspire further studies toward understanding the nature of conductive polymers at the atomic scale.
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2. |
- Li, Qing, et al.
(author)
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Hierarchical Dehydrogenation Reactions on a Copper Surface
- 2018
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In: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 140:19, s. 6076-6082
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Journal article (peer-reviewed)abstract
- Hierarchical control of chemical reactions is being considered as one of the most ambitious and challenging topics in modern organic chemistry. In this study, we have realized the one-by-one scission of the X-H bonds (X = N and C) of aromatic amines in a controlled fashion on the Cu(lll) surface. Each dehydrogenation reaction leads to certain metal-organic supramolecular structures, which were monitored in single-bond resolution via scanning tunneling microscopy and noncontact atomic force microscopy. Moreover, the reaction pathways were elucidated from X-ray photoelectron spectroscopy measurements and density functional theory calculations. Our insights pave the way for connecting molecules into complex structures in a more reliable and predictable manner, utilizing carefully tuned stepwise on-surface synthesis protocols.
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3. |
- Tian, Chen, et al.
(author)
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An effective modulation of bulk perovskite by V2CTx nanosheets for efficient planar perovskite solar cells
- 2023
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In: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 11:10, s. 5015-5026
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Journal article (peer-reviewed)abstract
- Crystallization modulation and defect passivation are key for high performance perovskite solar cells (PSCs) through suppressing defects in the surface and/or near the grain boundaries (GBs) of solution-processed perovskite films. In this work, we report simultaneous modulation of crystallization and passivation of defects for perovskites through a new vanadium carbide (V2CTx) MXene that is employed in an anti-solvent. The final modified perovskite film showed an improved crystallization, better energy level alignment and higher hole injection with a hole-transporting layer, leading to an increased power conversion efficiency from 20.1% up to 23.47% for planar PSCs, with enhanced device stability retaining over 90% of the initial PCE after 1000 hours exposure under 40-60% relative humidity at 25 degrees C. We have further employed the synchrotron radiation in situ grazing-incidence wide-angle X-ray scattering (GIWAXS) equipment to monitor the kinetic process of crystallization during spin-coating; it is notable that a lower dimensional perovskite structure (n < 3) was observed in the modified perovskite film during the process of dropping the antisolvent CB with V2CTx, which helps explain the enhanced device stability.
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