Macroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting

Lin, Jingkai; Wang, Yantao; Tian, Wenjie; Zhang, Huayang; Sun, Hongqi; Wang, Shaobin

doi:10.1021/acscatal.3c02076

Cited by 15 publications

(10 citation statements)

References 61 publications

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“…Carbon-based materials, such as carbon nanotubes (CNTs), ,, graphene, , graphitic carbon nitride (g-C 3 N 4 ), , and carbon quantum dots, are extensively used for catalytic hydrogen production (see Table ). Through precise structural engineering and surface modifications, carbon materials with higher surface areas and significant pore volumes have found widespread applications in various catalytic processes.…”

Section: Various Catalysts Used For Hydrogen Generationmentioning

confidence: 99%

Review and Outlook of Hydrogen Production through Catalytic Processes

Kumar,

Singh,

Dutta

2024

Energy Fuels

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Hydrogen holds immense potential as a sustainable energy source as a result of its eco-friendliness and high energy density. Thus, hydrogen can solve the energy and environmental challenges. However, it is crucial to produce hydrogen using sustainable approaches in a cost-efficient manner. Currently, hydrogen can be produced by utilizing diverse feedstocks, such as natural gas, methane, ammonia, smaller organic molecules (methanol, ethanol, glycerol, and formic acid), biomass, and water. These feedstocks undergo conversion into hydrogen through different catalytic processes, including steam reforming, pyrolysis, catalytic decomposition, gasification, electrolysis, and photoassisted methods (photoelectrochemical, photocatalysis, and biophotolysis). Researchers have extensively explored various catalysts, including metals, alloys, oxides, non-oxides, carbon-based materials, and metal−organic frameworks, for these catalytic methods. The primary objectives have been to attain higher activity, selectivity, stability, and cost effectiveness in hydrogen generation. The efficacy of these catalytic processes is significantly dependent upon the performance of the catalysts, emphasizing the need for further research and development to create more efficient catalysts. However, during catalytic hydrogen production, gases like CO 2 , O 2 , CO, N 2 , etc. are produced alongside hydrogen. Separation techniques, such as pressure swing adsorption, metal hydride separation, and membrane separation, are employed to obtain high-purity hydrogen. Furthermore, a techno-economic analysis indicates that catalytic hydrogen production through steam reforming of natural gas/methane is currently viable and commercially successful. Photovoltaic electrolysis has been commercialized, but the cost of hydrogen production is still higher. Meanwhile, other photoassisted methods are in the development phase and hold the potential for future commercialization.

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Section: Various Catalysts Used For Hydrogen Generationmentioning

confidence: 99%

Review and Outlook of Hydrogen Production through Catalytic Processes

Kumar,

Singh,

Dutta

2024

Energy Fuels

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“…13 Heteroatom doping induces localized midgap states in the interband region that can accommodate photoexcited electrons from VB, allowing the absorption of photons with energy lower than its intrinsic band gap. 4,30 However, the positively shifted midgap state may lead to the excitation of hot electrons with ineffective energy, which is unfavorable for reactivity. 4,31…”

Section: Band Structurementioning

confidence: 99%

“…4,30 However, the positively shifted midgap state may lead to the excitation of hot electrons with ineffective energy, which is unfavorable for reactivity. 4,31…”

Section: Band Structurementioning

confidence: 99%

“…Hybridizing C/N orbitals in CN with foreign elements can reorient orbitals and redistribute charges, optimizing its functionality. 4,32 Generally, orbital hybridization is feasible only if the substrate orbitals possess similar energies to those of the foreign species. 32 Because CN usually serves as a support to accommodate metal-based species (e.g., single atoms, nanoclusters, and nanoparticles), 10,20 the hybridization of metal d and C/N sp orbitals dominates the electron structure.…”

Section: Dos and Orbital Hybridizationmentioning

confidence: 99%

“…2023, 13, 11711−11722. 4 This research displayed an innovative silica-template-assisted pyrolysis strategy to prepare carbon nitride-supported single-atom Ni catalysts for photocatalytic NH 3 splitting. Ni−N 4 induced orbital reorientation and charge redistribution, optimizing the adsorption and dissociation of reaction intermediates in the NH 3 splitting reaction.…”

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confidence: 99%

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Electronic Structure and Functions of Carbon Nitride in Frontier Green Catalysis

Lin,

Tian,

Zhang

et al. 2024

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: Graphitic carbon nitride-based materials have emerged as promising photocatalysts for a variety of energy and environmental applications owing to their "earth-abundant" nature, structural versatility, tunable electronic and optical properties, and chemical stability. Optimizing carbon nitride's physicochemical properties encompasses a variety of approaches, including the regulation of inherent structural defects, morphology control, heterostructure construction, and heteroatom and metal-atom doping. These strategies are pivotal in ultimately enhancing their photocatalytic activities. Previous reviews with extensive examples have mainly focused on the synthesis, modification, and application of carbon nitride-based materials in photocatalysis. However, there has been a lack of straightforward and in-depth discussion to understand the electronic characteristics and functions of various engineered carbon nitrides as well as their precise tailoring strategies and ultimately to explain the regularity and specificity of their improved performance in targeted photocatalytic systems. In the past ten years, our group has conducted extensive investigations on carbon nitride-based materials and their application in photocatalysis. These studies demonstrate the close yet intricate relationship between the electronic structure of carbon nitride materials and their photocatalytic reactivity. Understanding the electronic structure and functions of carbon nitride, as well as different engineering strategies, is essential for the improvement of photocatalytic processes from fundamental study to practical applications.To this end, in this Account, we first delve into the nature of the electronic properties of carbon nitride, highlighting the electronic structures, including band structure, density of states, molecular orbitals, and band center, as well as its electronic functions, such as the charge distribution, internal electric field, and external electric force. Subsequently, based on recent research in our group, we present a detailed discussion of the strategic modifications of carbon nitride and the consequential impacts on the physicochemical properties, particularly the optical properties and intrinsic electronic characteristics, for enhancing the photocatalytic performance. These modifications are categorized as follows: (i) component changing, which involves intralayer and interface heterojunctions as well as homojunctions, to modulate the band-edge potentials and reactivity of photoinduced electrons and holes toward surface redox reactions; (ii) dimensional tuning, which engineers the dimensional structure of carbon nitride, to influence the electron transfer direction; (iii) defect and heteroatom modification, which introduces a symmetry break in the carbon nitride framework, to promote charge redistribution for altering the charge density and electronic structure; and (iv) anchoring of single-atom metals to facilitate orbital hybridization and charge transfer enhancem...

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Solar‐Driven Hydrogen Evolution from Value‐Added Waste Treatment

Yu,

Li,

Jiang

et al. 2024

Advanced Energy Materials

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Hydrogen is one of the most important energy alternatives to conventional fossil‐based fuel. Solar energy based photocatalytic hydrogen evolution (PHE) is a salient approach to produce hydrogen fuel but its efficiency is generally limited by the sluggish and energy‐unfavorable oxidation reaction. Meanwhile, waste treatment has become a worldwide problem and clean treatment is highly demanded to avoid the vast greenhouse emission currently. Inspiringly, PHE can be effectively coupled with the favorable photooxidation of many wastes, which kills two birds with one stone. In this review, the recent progress in PHE coupled with waste treatment is presented, where typical solid, liquid, and gas wastes have been briefly discussed. Focusing on the understanding of complicated reaction mechanism and the revelation of oxidation products, the cutting‐edge techniques for photophysics and surface chemistry characterization have been analyzed, which are imperative to facilitate the following investigation. Finally, the developing trend and existing issues in current research are also discussed in detail so that a holistic blueprint of PHE coupled with waste treatment can be portrayed to accelerate their application in a realistic world.

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Macroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting

Cited by 15 publications

References 61 publications

Review and Outlook of Hydrogen Production through Catalytic Processes

Review and Outlook of Hydrogen Production through Catalytic Processes

Electronic Structure and Functions of Carbon Nitride in Frontier Green Catalysis

Solar‐Driven Hydrogen Evolution from Value‐Added Waste Treatment

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