Insights into the Role of Protonation in Covalent Triazine Framework-Based Photocatalytic Hydrogen Evolution

Ye, Huan; Gong, Ning; Cao, Yaqi; Fan, Xiaobin; Song, Xiancheng; Li, Hao; Wang, Chi; Mei, Yi; Zhu, Yuanzhi

doi:10.1021/acs.chemmater.1c02697

Cited by 24 publications

(16 citation statements)

References 57 publications

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“…Total density of state (TDOS), partial density of state (PDOS), and overlap partial density of state (OPDOS) (significantly referred to from literatures as crystal orbital overlap population) diagrams were plotted (Figure S1), and analyzed with major interest on PDOS. This was created by entangling the molecular orbital information with Gaussian curves 39 of heights, and full width of 0.2 eV using multiwave-function software.…”

Section: Resultsmentioning

confidence: 99%

Electrocatalytic activity of metal encapsulated, doped, and engineered fullerene-based nanostructured materials towards hydrogen evolution reaction

Louis

Ikenyirimba

Unimuke

et al. 2022

Sci Rep

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The utilization of nanostructured materials as efficient catalyst for several processes has increased tremendously, and carbon-based nanostructured materials encompassing fullerene and its derivatives have been observed to possess enhanced catalytic activity when engineered with doping or decorated with metals, thus making them one of the most promising nanocage catalyst for hydrogen evolution reaction (HER) during electro-catalysis. Prompted by these, and the reported electrochemical, electronic and stability advantage, an attempt is put forward herein to inspect the metal encapsulated, doped, and decorated dependent HER activity of C 24 engineered nanostructured materials as effective electro-catalyst for HER. Density functional theory (DFT) calculations have been utilized to evaluate the catalytic hydrogen evolution reaction activity of four proposed bare systems: fullerene (C 24 ), calcium encapsulated fullerene (Ca enc C 24 ), nickel-doped calcium encapsulated fullerene (Ni dop Ca enc C 24 ), and silver decorated nickel-doped calcium encapsulated (Ag dec Ni dop Ca enc C 24 ) engineered nanostructured materials at the TPSSh/GenECP/6-311+G(d,p)/LanL2DZ level of theory. The obtained results divulged that, a potential decrease in energy gap (E gap ) occurred in the bare systems, while a sparing increase was observed upon adsorption of hydrogen onto the surfaces, these surfaces where also observed to maintain the least E H–L gap while the Ag dec Ni dop Ca enc C 24 surface exhibited an increased electrocatalytic activity when compared to others. The results also showed that the electronic properties of the systems evinced a correspondent result with their electrochemical properties, the Ag-decorated surface also exhibited a proficient adsorption energy and Gibb’s free energy (ΔG H ) value. The engineered Ag-decorated and Ni-doped systems were found to possess both good surface stability and excellent electro-catalytic property for HER activities.

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Section: Resultsmentioning

confidence: 99%

Electrocatalytic activity of metal encapsulated, doped, and engineered fullerene-based nanostructured materials towards hydrogen evolution reaction

Louis

Ikenyirimba

Unimuke

et al. 2022

Sci Rep

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“…Defects were mainly classified into four categories based on size: point defects, line defects, surface defects and bulk defects. Among them, point defects were a type of defect that deviates from the crystal structure or normal arrangement in the lattice nodes or adjacent microscopic regions, which were mainly classified into oxygen vacancies (OV), sulfur vacancies (SV) and nitrogen vacancies (NV) according to elemental categories [ 58 ]. Whether in photocatalysts or electrocatalysts, how to introduce oxygen vacancies (OVs)—which are anionic vacancies with a low free-energy formation and are usually easily formed in transition metal oxides—is the topic that is most studied.…”

Section: Modification Strategies For the Photo(electro)catalystsmentioning

confidence: 99%

Advances in Semiconductor-Based Nanocomposite Photo(electro)catalysts for Nitrogen Reduction to Ammonia

Zuo

2023

Molecules

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Photo(electro)catalytic nitrogen fixation technology is a promising ammonia synthesis technology using clean solar and electric energy as the driving energy. Abundant nitrogen and water as raw materials uphold the principle of green and sustainable development. However, the generally low efficiency of the nitrogen reduction reaction has seriously restricted the application and development of this technology. The paper introduces the nitrogen reduction process and discusses the main challenges and differences in the current photo(electro)catalytic nitrogen fixation systems. It focuses on promoting the adsorption and activation of N2 and the resolution and diffusion of NH3 generated. In recent years, reviews of the modification strategies of semiconductor materials in light of the typical cases of nitrogen fixation have been reported in the literature. Finally, the future development trend of this field is analyzed and prospected.

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“…The protonated CTF-1 presented a contact angle of 38.4°, which was only one-third of the bare sample, resulting in ca. 10 times enhancement of the hydrogen evolution rate [ 51 ].…”

Section: Optimization Of Ctfs For Photocatalytic Hydrogen Generationmentioning

confidence: 99%

Modification of Covalent Triazine-Based Frameworks for Photocatalytic Hydrogen Generation

2022

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The conversion of solar energy and water to hydrogen via semiconductor photocatalysts is one of the efficient strategies to mitigate the energy and environmental crisis. Conjugated polymeric photocatalysts have advantages over their inorganic counterparts. Their molecular structures, band structures, and electronic properties are easily tunable through molecular engineering to extend their spectral response ranges, improve their quantum efficiencies, and enhance their hydrogen evolution rates. In particular, covalent triazine-based frameworks (CTFs) present a strong potential for solar-driven hydrogen generation due to their large continuous π-conjugated structure, high thermal and chemical stability, and efficient charge transfer and separation capability. Herein, synthesis strategies, functional optimization, and applications in the photocatalytic hydrogen evolution of CTFs since the first investigation are reviewed. Finally, the challenges of hydrogen generation for CTFs are summarized, and the direction of material modifications is proposed.

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Insights into the Role of Protonation in Covalent Triazine Framework-Based Photocatalytic Hydrogen Evolution

Cited by 24 publications

References 57 publications

Electrocatalytic activity of metal encapsulated, doped, and engineered fullerene-based nanostructured materials towards hydrogen evolution reaction

Electrocatalytic activity of metal encapsulated, doped, and engineered fullerene-based nanostructured materials towards hydrogen evolution reaction

Advances in Semiconductor-Based Nanocomposite Photo(electro)catalysts for Nitrogen Reduction to Ammonia

Modification of Covalent Triazine-Based Frameworks for Photocatalytic Hydrogen Generation

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