Thermally Induced Dehydrogenative Coupling of Organosilanes and H-Terminated Silicon Quantum Dots onto Germanane Surfaces

Yu, Haoyang; Thiessen, Alyxandra; Hossain, Asjad; Kloberg, Marc Julian; Rieger, Bernhard; Veinot, Jonathan G. C.

doi:10.1021/acs.chemmater.0c00482

Cited by 11 publications

(36 citation statements)

References 35 publications

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“…These high M w values are certainly a reflection limited solution compatibility of the present (GeH 2 ) n , and drawing any conclusions from this data beyond that both molecular weights are large is ill-advised. While limited cross-linking of polymer chains via the formation of Ge–Ge bonds within the present (GeH 2 ) n agglomerates cannot be fully neglected, such reactions are unexpected and have not been noted for analogous approaches that yield germanane (i.e., H-terminated Ge nanosheets) from the CaGe 2 Zintl phase. , Furthermore, the likelihood of homonuclear dehydrocoupling reactions of Ge–H moieties on different (GeH 2 ) n chains in the absence of substantial heating and/or transition metal catalysts is extremely unlikely. , …”

Section: Resultsmentioning

confidence: 92%

“…28,30 Furthermore, the likelihood of homonuclear dehydrocoupling reactions of Ge−H moieties on different (GeH 2 ) n chains in the absence of substantial heating and/or transition metal catalysts is extremely unlikely. 37,38 XPS provides information regarding the elements present within a given material, as well as their corresponding bonding environments and oxidation states. Unfortunately, this analysis was not possible of the (GeH 2 ) n obtained from Method 1 because of its noted sensitivity, however we gained valuable insight into the composition of the (GeH 2 ) n provided by Method 2.…”

Section: Resultsmentioning

confidence: 99%

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Synthesis, Properties, and Derivatization of Poly(dihydrogermane): A Germanium-Based Polyethylene Analogue

Thiessen

et al. 2021

ACS Nano

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Polygermanes are germanium-based analogues of polyolefins and possess polymer backbones made up catenated Ge atoms. In the present contribution we report the preparation of a stable germanium polyethylene analogue -polydihydrogermane (i.e., (GeH2)n) -via two straightforward approaches that involve topotactic deintercalation of the CaGe Zintl phase. The resulting (GeH2)n possess morphologically dependent chemical and electronic properties and thermally decompose to yield amorphous hydrogenated Ge. We also show that the resulting (GeH2)n provide a platform from which functionalized polygermanes can be prepared via thermally-induced hydrogermylation-mediated pendant group substitution. This facile one-step derivatization reaction exploits Ge-H reactivity and opens the door to a wide array of tailored functional polygermanes.

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Section: Resultsmentioning

confidence: 92%

Section: Resultsmentioning

confidence: 99%

Synthesis, Properties, and Derivatization of Poly(dihydrogermane): A Germanium-Based Polyethylene Analogue

Thiessen

et al. 2021

ACS Nano

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“…Drawing on the work by Yu et al., we employed thermally induced dehydrogenative coupling to tether SiQDs to the surfaces of silicane (i.e., silicon nanosheets; SiNSs). [ 34 ] Subsequently, trimethyl(vinyl)silane (TMVS) was introduced to the exposed surfaces of the SiNS‐bonded SiQDs using established hydrosilylation protocols ( Scheme ). The resulting material (denoted TMVS‐SiQD@SiNS‐TMVS) did not render clear colloidal dispersions—as is usually the case for 3 nm SiQDs—and it no longer exhibited visible PL characteristic of the SiQDs (≈720 nm) [ 3 ] or SiNSs (≈515 nm) [ 33 ] ( Figure a, left).…”

Section: Resultsmentioning

confidence: 99%

“…The procedure used an adapted literature‐known method to deposit silicon nanocrystals (SiQD‐H) on silicane (SiNS‐H). [ 34 ] The subsequent hydrosilylations use established methods to modify the SiQDs’ surface with desired alkenes. [ 35,49 ]…”

Section: Methodsmentioning

confidence: 99%

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Surface‐Anisotropic Janus Silicon Quantum Dots via Masking on 2D Silicon Nanosheets

Kloberg

Groß

et al. 2021

Advanced Materials

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Surface‐anisotropic nanoparticles represent a new class of materials that shows potential in a variety of applications, including self‐assembly, microelectronics, and biology. Here, the first synthesis of surface‐anisotropic silicon quantum dots (SiQDs), obtained through masking on 2D silicon nanosheets, is presented. SiQDs are deposited on the 2D substrate, thereby exposing only one side of the QDs, which is functionalized through well‐established hydrosilylation procedures. The UV‐sensitive masking substrate is removed through UV‐irradiation, which simultaneously initiates the hydrosilylation of a second substrate, thereby introducing a second functional group to the other side of the now free‐standing SiQDs. This renders surface‐anisotropic SiQDs that have two different functional groups on either side of the particle. This method can be used to introduce a variety of functional groups including hydrophilic and hydrophobic substrates, while the unique optoelectronic properties of the SiQDs remain unaffected. The anisotropic morphology of the QDs is confirmed through the aggregation behavior of amphiphilic Janus SiQDs at the interface of water and hexane. Additionally, anisotropic SiQDs are used to produce the first controlled (sub)monolayer of SiQDs on a gold wafer.

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Faster and Safer “In situ” Synthesis of Germanane and Silicane

Georgantas,

Giousis,

Moissinac

et al. 2024

Small Methods

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Germanane (GeH) and silicane (SiH), members of the Xanes family, have garnered significant attention as 2D materials due to their diverse properties, which hold promise for applications in electronics, optoelectronics, energy storage, and sensing. Typically, highly concentrated hydrochloric acid (HCl) or hydrofluoric acid (HF) is employed in the synthesis of these Xanes, but both routes are problematic due to slow kinetics and safety concerns, respectively. Here for the first time, a faster and safer method is demonstrated for Xanes synthesis that harnesses the generation of HF “in situ” using a solution of HCl and lithium fluoride (LiF) salt, overcoming the key challenges of the conventional methods. A variety of characterization techniques to establish a baseline is utilized for both Xanes and to provide a holistic knowledge regarding this method, the possible consequences of this approach, and the possibility of applying it to other layered Zintl phases. The novel synthesis protocol results in high‐quality GeH and SiH with bandgaps (Eg) of 1.75 and 2.47 eV respectively, highlighting their potential suitability for integration into semiconductor applications.

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Thermally Induced Dehydrogenative Coupling of Organosilanes and H-Terminated Silicon Quantum Dots onto Germanane Surfaces

Cited by 11 publications

References 35 publications

Synthesis, Properties, and Derivatization of Poly(dihydrogermane): A Germanium-Based Polyethylene Analogue

Synthesis, Properties, and Derivatization of Poly(dihydrogermane): A Germanium-Based Polyethylene Analogue

Surface‐Anisotropic Janus Silicon Quantum Dots via Masking on 2D Silicon Nanosheets

Faster and Safer “In situ” Synthesis of Germanane and Silicane

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