Covalent grafting of molecular catalysts on C3NxHy as robust, efficient and well-defined photocatalysts for solar fuel synthesis

Windle, Christopher D.; Wieczorek, Alexander; Xiong, Lunqiao; Sachs, Michael L.; Bozal‐Ginesta, Carlota; Cha, Hyojung; Cockcroft, Jeremy K.; Durrant, James R.; Tang, Junwang

doi:10.1039/d0sc02986f

Cited by 15 publications

(10 citation statements)

References 35 publications

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“…These CN‐catalyst hybrid materials, namely CN urea ‐Ni(abt) 2 , CN DCDA ‐Ni(abt) 2 , FAT‐Ni(abt) 2 , and ONLH‐Ni(abt) 2 , were formed as a result of the coupling of aryl amines and aryl chlorides in the presence of potassium tert ‐butoxide catalyst ( Figure ). [ 79 ] The CN‐catalyst materials exhibited over 8 days of hydrogen evolution, rapid and lasting charge separation, and photoactivity under irradiation of 475 nm light. Although the surface area was found to be related to catalyst loading, the lowest loading was observed for CN DCDA that had a surface area higher than FAT.…”

Section: Surface Functionalization Of G‐c3n4mentioning

confidence: 99%

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Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Fidan

Torabfam

Saleem

et al. 2021

Adv Energy and Sustain Res

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Graphitic carbon nitride (g‐C3N4) is a metal‐free semiconductor that has been widely regarded as a promising candidate for sustainable energy production or storage. In recent years, g‐C3N4 has become the center of attention by virtue of its impressive properties, such as being inexpensive, easily fabricable, nontoxic, highly stable, and environment friendly. Herein, the recent research developments related to g‐C3N4 are outlined, which sheds light on its future prospective. Various synthetic methods and their impact on the properties of g‐C3N4 are detailed, along with discussion on frequently used characterization methods. Different approaches for g‐C3N4 surface functionalization, mainly categorized under covalent and noncovalent strategies, are outlined. Moreover, the processing methods of g‐C3N4, such as g‐C3N4‐based thin films, hierarchical, and hybrid structures, are explored. Next, compared with the extensively studied energy‐related applications of the modified g‐C3N4s, relatively less‐examined areas, such as environmental and sensing, are presented. By highlighting the strong potential of these materials and the existing research gaps, new researchers are encouraged to produce functional g‐C3N4‐based materials using diverse surface modification and processing routes.

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Section: Surface Functionalization Of G‐c3n4mentioning

confidence: 99%

Section: Surface Functionalization Of G‐c3n4mentioning

confidence: 99%

Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Fidan

Torabfam

Saleem

et al. 2021

Adv Energy and Sustain Res

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“…Solar-hydrogen conversion has been an active research field. − Among the various developed technologies, the photocatalytic water-splitting technique for producing the clean and renewable hydrogen in a facile and ecofriendly process is considered to be a promising strategy for future energy supply. , So far, photocatalysts developed for photocatalytic H 2 evolution are generally inorganic semiconductors consisting of d 0 transition or d 10 post-transition-metal cations and group VA or VIA anions, , for instance, TiO 2 , GaN, CdS, and BiVO 4 . However, their photoactivities are not ideal, because of the low utilization of visible light (44% of the actual solar light spectrum), photocorrosion, and the presence of noble or toxic metals could be a severe barrier to the industrial application .…”

Section: Introductionmentioning

confidence: 99%

Controlled Synthesis of Nitro-Terminated Poly[2-(3-thienyl)-ethanol]/g-C₃N₄ Nanosheet Heterojunctions for Efficient Visible-Light Photocatalytic Hydrogen Evolution

Zhao

Kang

et al. 2021

ACS Sustainable Chem. Eng.

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Exploration of closely contacted polymeric nanoheterojunctions with suitable frontier molecular orbital energy levels is highly desired for promoting the carrier separation and further improving the photocatalytic performance. In our work, poly [2-(3-thienyl)ethanol]/g-C 3 N 4 (PTEtOH/g-C 3 N 4 ) nanosheet heterojunctions were successfully fabricated using a controlled surface hydroxyl-induced assembly process and displayed obviously improved visible-light performance for H 2 evolution. As verified by time-resolved photoluminescence spectra, surface photovoltage spectra and •OH amount measurements, the improved performance is due to the promoted photogenerated carrier transfer and separation in the synthesized PTEtOH/g-C 3 N 4 heterojunction with strengthened interface contacts via hydrogen bonding. Furthermore, single-wavelength photocurrent action spectra were performed to confirm that the promoted photogenerated carrier separation is mainly dependent on the excited high-level electron transfer from g-C 3 N 4 to PTEtOH. Interestingly, the photocatalytic performance is further improved by synthesizing nitro-terminated PTEtOH (N-PTEtOH) with lowered LUMO energy level and decreased particle size and then constructing N-PTEtOH/g-C 3 N 4 nanosheet heterojunction, exhibiting a factor-of-15 enhancement, in comparison with that of g-C 3 N 4 and obvious superiority to reported photoactivities. Noteworthily, abundant hydroxyl groups on the surface of the heterojunctions are beneficial for the uniform deposition of Pt nanoparticles as co-catalysts and hence for photocatalytic reactions. This study offers a feasible strategy to design efficient polymeric heterojunctions as nanophotocatalysts for solar-lightdriven energy production.

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“…For example, heteroatom doping (such as with boron, [10] fluorine, [11] sulfur, [12] phosphorus, [13] etc. ), surface morphology modification, [14] covalent attachment of molecules, [15] hybrid copolymerization, [16] exfoliation, [17] and heterojunction [18] have been used to overcome these obstacles. Among them, loading precious metals into CN to build a heterojunction is the most effective and simple strategy, because it has the advantages of restraining the recombination of carriers and adjusting the bandgap.…”

Section: Introductionmentioning

confidence: 99%

Hollow Carbon Sphere‐Modified Graphitic Carbon Nitride for Efficient Photocatalytic H₂ Production

Xiong

Luo

et al. 2021

Chemistry A European J

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A novel hybrid photocatalyst composed of hollow carbon nanospheres (NCS) and graphitic carbon nitride (CN) curly nanosheets has been prepared by the calcination of a NCS precursor and freeze‐dried urea. The optimized photocatalyst exhibits an efficient photocatalytic performance under visible light irradiation with a highest H2 generation rate of 3612.3 μmol g−1 h−1, leading to an apparent quantum yield of 10.04 % at 420 nm, five times higher than the widely reported benchmark photocatalyst CN (2.01 % AQY). The materials characterization shows that NCS‐modified CN curly nanosheets can promote photoelectron transfer and suppress charge recombination through their special coupling interface and NCS as an electron acceptor, which significantly improves the photocatalytic efficiency. Thus, this study provides an efficient strategy for the design of highly efficient photocatalyst, particularly suitable for a totally metal‐free photocatalytic system.

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Covalent grafting of molecular catalysts on C₃N_xH_y as robust, efficient and well-defined photocatalysts for solar fuel synthesis

Abstract: A nickel bis-aminothiophenol catalyst grafted onto a 2D carbon-nitride photocatalytically produces H2 beyond 8 days with turnover numbers reaching 1360.

Cited by 15 publications

References 35 publications

Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Controlled Synthesis of Nitro-Terminated Poly[2-(3-thienyl)-ethanol]/g-C₃N₄ Nanosheet Heterojunctions for Efficient Visible-Light Photocatalytic Hydrogen Evolution

Hollow Carbon Sphere‐Modified Graphitic Carbon Nitride for Efficient Photocatalytic H₂ Production

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Covalent grafting of molecular catalysts on C3NxHy as robust, efficient and well-defined photocatalysts for solar fuel synthesis

Abstract: A nickel bis-aminothiophenol catalyst grafted onto a 2D carbon-nitride photocatalytically produces H2 beyond 8 days with turnover numbers reaching 1360.

Cited by 15 publications

References 35 publications

Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Functionalized Graphitic Carbon Nitrides for Environmental and Sensing Applications

Controlled Synthesis of Nitro-Terminated Poly[2-(3-thienyl)-ethanol]/g-C3N4 Nanosheet Heterojunctions for Efficient Visible-Light Photocatalytic Hydrogen Evolution

Hollow Carbon Sphere‐Modified Graphitic Carbon Nitride for Efficient Photocatalytic H2 Production

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Covalent grafting of molecular catalysts on C₃N_xH_y as robust, efficient and well-defined photocatalysts for solar fuel synthesis

Controlled Synthesis of Nitro-Terminated Poly[2-(3-thienyl)-ethanol]/g-C₃N₄ Nanosheet Heterojunctions for Efficient Visible-Light Photocatalytic Hydrogen Evolution

Hollow Carbon Sphere‐Modified Graphitic Carbon Nitride for Efficient Photocatalytic H₂ Production