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Hydrogen self-supplying initiators excited by visible light for the fabrication of transparent films

Science China Chemistry 2024年第11期67卷 3868-3874页

作者： Qingze Pan Chiheng Liu Wenzhe Qiao Jianwei Li Saihe Yang Yangyang Xin Pengzhong Chen Jiangli Fan Xiaojun Peng State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical EngineeringDalian University of TechnologyDalian 116024China Ningbo Institute of Dalian University of Technology Ningbo 315016China Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China Liaoning Binhai Laboratory Dalian 116023China

Unimolecular Type Ⅱ radical photoinitiators(PIs) have received significant attention in photocuring owing to the fact that they improve the sustainability of the overall process compared with traditional Type Ⅱ radical photoinitiators. However, the photopolymerization efficiency of unimolecular Type Ⅱ radical photoinitiators is hindered by their short excitation wavelengths,poor photon capture abilities, and inefficient photobleaching performance. Herein, we report a coumarin-based self-sufficient initiator(C-NA), which is designed by integrating “hydrogen donor” and “hydrogen acceptor” into the coumarin framework and used for single-component visible light curing. C-NA exhibits a visible light absorbance and high molar extinction coefficient and is completely photobleached under the irradiation of 405 nm light-emitting diodes(LEDs). The formation of free radicals arises from the transfer of hydrogen from the diethylamino group to the coumarin framework, together with a highly efficient photodegradation process of C-NA. Finally, C-NA was successfully applied to prepare a transparent film material. Therefore,C-NA offers new insights into the design of promising unimolecular Type Ⅱ radical photoinitiators for photocuring.

关键词： photocuring photoinitiator hydrogen transfer visible light unimolecular photobleaching

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Highly dispersed Pt clusters encapsulated in MIL-125-NH_(2) via in situ auto-reduction method for photocatalytic H_(2) production under visible light

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Nano Research 2021年第11期14卷 4250-4257页

作者： Xiubing Huang Xiangjun Li Qingjie Luan Kaiyue Zhang Zhenyu Wu Baozhen Li Zuoshuai Xi Wenjun Dong Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing10083China

Efficient hydrogen production via photocatalysis with high utilization efficiency of Pt cocatalyst is of great importance for sustainable development. In this work, we report an in situ auto-reduction strategy to encapsulate highly dispersed Pt clusters inside the cages of MIL-125-NH_(2). The amino groups in MIL-125-NH_(2) first react with formaldehyde to form reducing groups (i.e.,–NH-CH_(2)OH), which can in situ auto-reduce the confined Pt^(2+) ions to ultrasmall Pt clusters within the cavities. With optimized Pt content, photocatalytic H_(2) production over the obtained Pt(1.5)/MIL-125-NH-CH_(2)OH catalyst with 1.43 wt.% Pt loading achieved as high as 4,496.4 µmol·g^(-1)·h^(-1) under visible light (λ > 420 nm) due to the facilitated transfer and separation of the photo-induced charger carriers arising from the synergetic effects between highly dispersed Pt clusters and MIL-125-NH-CH_(2)OH framework. This in situ auto-reduction strategy may be extended to encapsulate various kinds of metal or alloy clusters/nanoparticles within amino-functioned metal-organic frameworks (MOFs) with superior properties and excellent performance.

关键词： Pt clusters MIL-125-NH_(2) in situ auto-reduction method photocatalytic H_(2)production visible light

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N-doped NaTaO3 synthesized from a hydrothermal method for photocatalytic water splitting under visible light irradiation

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Journal of Energy Chemistry 2017年第3期26卷 515-521页

作者： Che-Chia Hu Hui-Hsin Huang Yu-Chi Huang Department of Chemical Engineering and R&D Center for Membrane Technology Chung Yuan Christian UniversityTaoyuan City 32023TaiwanChina

NaTaONcatalysts were synthesized by a hydrothermal（H） and a solid-state（S） methods in this *** H-and S-NaTaONsamples were characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM）, transmission electron microscopy（TEM）, UV–visible（UV–vis） diffuse reflectance spectroscopy, and photoluminescence（PL） spectroscopy. The XRD patterns of the H-and S-samples showed peaks indexed to the pure phase of perovskite NaTaOand minor peaks assignable to TaNat various synthesis temperatures. Substitution of oxygen by nitrogen ions causes the light absorption of the H-and S-NaTaONsamples to be extended to the 600–650 nm region, thus making the samples visible-light active. The NaTaONsamples exhibited photocatalytic activity for Hand Oevolution from aqueous methanol and silver nitrate solutions under visible-light irradiation. The UV–vis and PL spectra of the Hand S-catalysts revealed the presence of cationic vacancies and reduced metallic species, which acted as recombination centers. These results demonstrated that the preparation method plays a critical role in the formation of defect states, thereby governing the photocatalytic activity of the NaTaONcatalysts.

关键词： Photocatalysis H2 production N-doped NaTaO3 Hydrothermal method visible light

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Metal-organic frameworks incorporated with C3N4:A visible light enhanced platform for degradation of polybromodiphenyl ethers

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Journal of Environmental Sciences 2023年第12期134卷 44-54页

作者： Akese Emmanuel Meiying Yang Tingting Xu Qi Shen Chunyan Sun School of Chemistry and Chemical Engineering Shaoxing UniversityShaoxing 312000China School of Chemistry and Chemical Engineering Institute of New EnergyShaoxing UniversityShaoxing 312000China

A series of nano-photocatalysts metal-organic frameworks(MOFs)/graphitic carbon nitride(CN)(named MOFCN-x) with high activity have been synthesized by in-situ growth *** visible light irradiation, MOFCN-x hybrids show enhanced photocatalytic activity for the debromination of polybromodiphenyl ethers(PBDEs) compared with CN. Among all the hybrids, MOFCN-2 shows the highest reaction rate, which is 3.3 times as high as that in CN. MOFCN-x photocatalysts own stable visible light activity after recycled experiment. It indicates that a moderate amount of MOFs in MOFCN-x can largely enhance the photocatalytic ability by improved visible light absorption, larger specific surface area and better photo-generated charge carriers separation and transfer capabilities. More interestingly,the debromination pathway of PBDEs by MOFCN-x shows obvious selectivity compared with pure CN that bromines at meta-positions are much more susceptible than those at the paraand ortho-positions. The possible photoreductive mechanism has been proposed. This study shows that nanocomposite MOFCN can be an excellent candidate for dealing with halogen pollutants by solar-driven.

关键词： Graphitic carbon nitride Metal-organic frameworks Photocatalytic reduction Polybromodiphenyl ethers visible light

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Lanthanum and boron co-doped BiVO_4 with enhanced visible light photocatalytic activity for degradation of methyl orange

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Journal of Rare Earths 2013年第9期31卷 878-884页

作者：王敏车寅生牛超党明岩董多 College of Environmental and Chemical Engineering Shenyang Ligong University

BiVO4 photocatalysts co-doped with La and B were prepared by sol-gel method using citric acid as chelate. The samples were characterized by X-ray photoelectron spectroscopy （XPS）, X-ray diffraction （XRD）, scanning electron microscopy （SEM）, Bru-mauer-Emmett-Teller （BET）, UV-Vis diffuse reflectance spectra （DRS） and the photocatalytic activity was investigated by photo-catalytic degradation of methyl orange （MO）. The results showed that boron and lanthanum ions incorporated into the lattice of BiVO4, and co-doping led to more surface oxygen vacancies, high specific surface areas, small crystallite size, narrow band gap and intense light absorbance in visible region. And the doped La（III） ions could help the separation of photogenerated electrons. Com-pared with BiVO4 and B-BiVO4, the photocatalytic activity of La-B co-doped BiVO4 was remarkably improved due to the synergistic effects of the co-doped ions. The degradation rate of MO in 60 min was 98.4%when La doping content was 0.05 mol.%, which was much higher than that of pure BiVO4（20%） and B-BiVO4（37%）.

关键词： La-B-codoped BiVO4 photocatalyst visible light methyl orange solution rare earths

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In situ preparation of g-C3N4/Bi4O5I2 complex and its elevated photoactivity in Methyl Orange degradation under visible light

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Journal of Environmental Sciences 2020年第1期32卷 149-162页

作者： Zhe Feng Lin Zeng Qingle Zhang Shifeng Ge Xinyue Zhao Hongjun Lin Yiming He Department of Materials Science and Engineering Zhejiang Normal UniversityJinhua 321004China College of Chemistry and Life Sciences Zhejiang Normal UniversityJinhua 321004China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

A graphite carbon nitride(g-C3N4)modified Bi4O5I2 composite was successfully prepared insitu via the thermal treatment of a g-C3N4/Bi OI precursor at 400°C for 3 *** as-prepared g-C3N4/Bi4O5I2 showed high photocatalytic performance in Methyl Orange(MO)degradation under visible *** best sample presented a degradation rate of 0.164 min^-1,which is 3.2 and 82 times as high as that of Bi4O5I2 and g-C3N4,*** g-C3N4/Bi4O5I2 was characterized by X-ray powder diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Raman,X-ray photoelectron spectroscopy(XPS),ultraviolet-visible diffuse reflectance spectra(DRS),electrochemical impedance spectroscopy(EIS)and transient photocurrent response in order to explain the enhanced *** indicated that the decoration with a small amount of g-C3N4 influenced the specific surface area only ***,the capability for absorbing visible light was improved measurably,which was beneficial to the MO *** top of that,a strong interaction between g-C3N4 and Bi4O5I2 was *** interplay promoted the formation of a favorable heterojunction structure and thereby enhanced the charge ***,the g-C3N4/Bi4O5I2 composite presented greater charge separation efficiency and much better photocatalytic performance than ***,g-C3N4/Bi4O5I2 also presented high stability.·O2^- and holes were verified to be the main reactive species.

关键词： g-C3N4 Bi4O5I2 Methyl Orange degradation Heterojunction visible light

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Development of Sn^(2+)-based oxyfluoride photocatalyst with visible light response of ca.650 nm via strengthened hybridization of Sn 5s and O 2p orbitals

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Journal of Energy Chemistry 2021年第12期30卷 385-390,I0009页

作者： Yanpei Luo Xin Zhou jiangwei Zhang Yu Qia Zheng Lia Fuxiang Zhang Can Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian National Laboratory for Clean EnergyThe Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)Dalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China College of Environment and Chemical Engineering Dalian UniversityDalian 116622LiaoningChina

The hybridization between the outmost s orbitals of metal(Bi^(3+),Sn^(2+),Pb^(2+),Ag^(+))and O 2 p orbitals has been widely employed to develop innovative semiconductors with upshift valence band as well as extended visible light response,but it is still challenging to obtain photocatalyst with absorption edge of above 550 *** we report a novel Sn^(2+)-based oxyfluoride Sn_(2)TiNbO_6 F(STNOF)photocatalyst with a pyrochlore structure to exhibit an extended absorption edge to 650 nm and dual functionalities of both water reduction and *** functional theory calculations suggest that the unprecedented broad-spectrum response of STNOF is mainly ascribed to the strengthened hybridization between O 2 p and Sn 5 s orbitals remarkably upshifting the valence band,which is caused by the distortion and compressive strain in the Sn06 F2 dodecahedron with second-order Jahn-Teller effect due to partial fluorine *** structural distortion and compressive strain are experimentally confirmed by the Fourier-transformed extended X-ray absorption fine *** probe tests of the photocatalytic functionalities,water reduction and oxidation half reactions were examined to see obvious H_(2)and O_(2)evolution under visible light *** work may provide an alternative strategy of developing extended visible light responsive semiconductors for promising solar energy conversion.

关键词： Photocatalyst visible light Water splitting DFT Structural characterizations

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Enhanced photocatalytic hydrogen evolution along with byproducts suppressing over Z-scheme CdxZn1-xS/Au/g-C3N4 photocatalysts under visible light

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Science Bulletin 2017年第9期62卷 602-609页

作者： He Zhao Xiaoling Ding Bing Zhang Yingxuan Li Chuanyi Wang Laboratory of Environmental Sdences and Technology Xinjiang Technical Institute of Physics & Chemistry Urumqi 830011 China Key Laboratory of Functional Materials and Devices for Special Environments Chinese Academy of Sciences Urumqi 830011 China University of Chinese Academy of Sciences Beijing 100049 China

Inspired by natural photosynthesis, a new series of Z-scheme Cd_xZn_(1-x)S/Au/g-C_3N_4 photocatalysts were synthesized via depositing Au particles on g-C_3N_4, followed by anchoring CdxZn_(1-x)S solid solution on the pre-formed Au/g-C_3N_4 for photocatalytic hydrogen evolution. Their structure, morphology and optical property were investigated in detail. Photocatalytic activities of the developed photocatalysts for water splitting were evaluated under visible-light irradiation(k > 420 nm) using glucose as electron *** highest hydrogen evolution rate of 123 lmol g^(-1)h^(-1)is achieved by Cd_(0.8Z)n_(0.2)S/Au/g-C_3N_4, which is 52.2 and 8.63 times higher than that of Au/g-C_3N_4 and Cd S/Au/g-C_3N_4, respectively. The results of photoluminescence spectra, photoelectrochemical and time-resolved photoluminescence spectra indicate that the improved photocatalytic activities for Cd_xZn_(1-x)S/Au/g-C_3N_4 are due to the efficient separation of photogenerated carriers. In addition, it is noteworthy that the undesired byproducts CO and CO_2 are greatly reduced by introducing CdxZn_(1-x)S over Au/g-C_3N_4 surface. In the photocatalytic process, gluconic acid originated from the reaction of photogenerated hydroxyl radical with glucose plays a vital role on suppressing the formation of the gas byproducts. The present work will provide a new strategy to design Z-scheme photocatalysts with enhanced efficiency for water splitting along with suppressing the byproducts.

关键词： Hydrogen evolution CdxZn1-xS/Au/g-C3N4 Byproducts Z-scheme visible light

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High efficiently harvesting visible light and vibration energy in(1−x)AgNbO_(3)-xLiTaO_(3) solid solution around antiferroelectric-ferroelectric phase boundary for dye degradation

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Journal of Advanced Ceramics 2022年第10期11卷 1641-1653页

作者： Tufeng HE Zhenzhu CAO Guorong LI Yanmin JIA Biaolin PENG College of Chemical Engineering Inner Mongolia University of TechnologyHohhot 010051China Key Laboratory of Inorganic Function Material and Device Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China School of Science Xi’an University of Posts&TelecommunicationsXi’an 710121China School of Advanced Materials and Nanotechnology Xidian UniversityXi’an 710126China

Simultaneously employing light and vibration energy by piezoelectric material to realize environmental remediation is an advanced oxidation *** niobate(AgNbO_(3))is a visible light driven photocatalyst for the removal of organic ***,the high recombination rate of photo-generated electrons and holes suppresses its photocatalytic *** potential excited by vibration can facilitate the separation of light induced ***,AgNbO_(3) is an *** this work,distinct photo-/vibration-bi-catalysis has been achieved in ferroelectric(1−x)AgNbO_(3)-xLiTaO_(3) solid *** results show that ~96% Rhodamine B(RhB)can be decomposed under the bi-excitation of ultrasound and visible light within 120 min with 0.95AgNbO_(3)-0.05LiTaO_(3) *** synergy effect from efficient visible light excitation and enhanced separation of the photo-induced charges from the electric field by the mechanical strain results in the distinct decomposition performance of catalysts.

关键词： piezoelectric effect photocatalysis visible light decomposition

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Deoxygenative alkylation of tertiary amides using alkyl iodides under visible light

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Science China Chemistry 2022年第11期65卷 2231-2237页

作者： Feng Zhao Feng Jiang Xiaoming Wang The Education Ministry Key Lab of Resource Chemistry and Shanghai Key Laboratory of Rare Earth Functional Materials College of Chemistry and Materials ScienceShanghai Normal UniversityShanghai 200234China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou310024China

It is an unceasing goal for organic chemists to develop new catalytic methodologies for functional group transformations of widespread molecular structures. Amides are readily available from simple and reliable reactions, which are common structural units found in biologically active compounds. Consequently, they are attractive to be exploited in amine synthesis by reductive cross coupling. However, deoxygenative functionalization of amides is a long-standing challenge owing to the inertness of the resonance-stabilized amide C=O bond. In this work, a deoxygenative alkylation strategy was demonstrated, which combines amides and alkyl iodides to build structurally diverse tertiary alkylamines in a single step. Compared with previous deoxygenative alkylation of amides using organometallic reagents as functional partner, this work uses stable and easily available alkyl halides as functionalization reagents. The versatile and flexible strategy plus structural and functional diversity of readily available amides and alkyl iodides renders it highly appealing for the streamlined synthesis of tertiary amines and would be of much interest in areas such as pharmaceutical and agrochemical research.

关键词： deoxygenative alkylation amide transformation alkyl radical alkylamine visible light

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