Article
Chemistry, Multidisciplinary
Xinye Liu, Bo Li, Wei Yang, Yang-Rong Yao, Le Yang, Jiaxin Zhuang, Xiaomeng Li, Peng Jin, Ning Chen
Summary: The chemical functionalization of actinide endohedral metallofullerenes was systematically investigated, revealing higher reactivity compared to their lanthanide analogs. The study successfully synthesized and characterized novel EMF derivatives, providing insights into their exceptional chemical properties and potential applications.
Article
Chemistry, Inorganic & Nuclear
Jia-Qi Song, Yu-Lin Lu, Shao-Zhe Yi, Jian-Hua Zhang, Mei Pan, Cheng-Yong Su
Summary: Photocatalytic reduction of excess CO2 in the atmosphere to value-added chemicals by visible light can be achieved using a trinuclear Re(I)-coordinated organic cage (Re-C-4(R)) as the supramolecular photocatalyst. The Re-C-4(R) exhibits higher catalytic activity and CO2 adsorption ability compared to its mononuclear analogue Re-bpy, due to its covalent linkage, cryptand structure, and multiple amine groups. The trinuclear cryptate structure of Re-C-4(R) also facilitates electron transfer efficiency during CO2 reduction, as indicated by its shorter decay lifetimes in transient absorption and photoluminescence decay spectra compared to Re-bpy.
INORGANIC CHEMISTRY
(2023)
Article
Polymer Science
Hongwei Lu, Jingfang Li, Tanlong Xue, Jun Nie, Xiaoqun Zhu
Summary: In this study, eight types of chalcone derivatives were synthesized, and their absorption wavelength and range were found to be influenced by the substituents. When the substituents were positioned on the same side, a stronger electron donor led to a longer maximum absorption wavelength. Among them, C4S showed the highest efficiency in photochemical hydrogen atom transfer, resulting in high polymerization efficiency. It also showed great potential for deep curing and curing of light-colored materials due to its lighter color and weaker visible light absorption.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Engineering, Environmental
Minglu Sun, Peng Zhou, Jiali Peng, Chuanshu He, Ye Du, Zhicheng Pan, Shijun Su, Fan Dong, Yang Liu, Bo Lai
Summary: By using rare earth oxide functionalized carbon nitride, photoexcited electron transfer can be mediated under visible light irradiation to boost PMS-based oxidation decontamination. This work reveals the mechanism and provides a new strategy for photocatalytic oxidation in environmental remediation.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Feng Zhang, Jun Ma, Ya Tan, Gang Yu, Hongxin Qin, Lirong Zheng, Hongbo Liu, Run Li
Summary: A porous organic cage is reported as a high-quality support for single metal atoms, showing extended visible light absorption, suppressed charge recombination, and improved electron transfer. The obtained single Co atoms anchored organic cage demonstrates excellent photocatalytic performance for oxidation of amines under visible light.
Article
Chemistry, Multidisciplinary
Hong-Lei Xu, Chad Studvick, Chao Liu, Yuan Xue, Ivan A. Popov, Zhong-Ming Sun
Summary: An unexpected single-metal-filled double-cage cluster has been reported, representing the largest group 14 intermetalloid cluster encapsulating a single transition metal atom. The structural characteristic of the cluster is described, and the deviation of the central atom is discussed in terms of vibronic coupling and pseudo-Jahn-Teller distortion.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Applied
Zhixiong Song, Shuwen Yu, Kaixian Wang, Zhengming Jiang, Liyan Xue, Fan Yang
Summary: A novel Sc-doped Bi3TiNbO9 ferroelectric nanofiber was fabricated by electrospinning. The nanofibers, with a diameter of approximately 100 nm, exhibited superior photocatalytic activity compared to powders prepared by the solid-state method, attributed to their high specific surface area and surface activity. The doping of Sc reduced the band gap of Bi3TiNbO9 and further enhanced the photocatalytic efficiency. The Bi3TiNbO9 nanofibers containing 5 mol% Sc showed the highest photocatalytic activity, degrading 98.55% of RhB under 405 nm light irradiation for 120 min. The nanofiber catalyst exhibited excellent stability with only a 2.42% decrease in degradation rate after three cycles of photocatalytic experiments. This work demonstrates the promising application of electrospinning technology in the field of photocatalysis.
JOURNAL OF RARE EARTHS
(2023)
Article
Chemistry, Multidisciplinary
Won Oh Choi, Young Jae Jung, Minyoung Kim, Hoyun Kim, Jingjing Li, Hyebin Ko, Hong-In Lee, Hye Jin Lee, Jungkyu K. Lee
Summary: This study demonstrated the effects of substituents in fluorescein on the photoredox catalytic performance under visible light. By characterizing the fluorescein derivatives and comparing the results of photopolymerization reactions, it was found that the amine and nitro groups had the largest impact on the performance, while other substituents also had some influence. These findings are important for the development of improved photoredox catalysts.
Article
Chemistry, Multidisciplinary
Xiahui Lin, Zidong Xie, Bo Su, Mei Zheng, Wenxin Dai, Yidong Hou, Zhengxin Ding, Wei Lin, Yuanxing Fang, Sibo Wang
Summary: Use of Co9S8 cages as a nonprecious cocatalyst for visible-light CO2 reduction has shown to accelerate charge separation, enhance CO2 activation, and efficiently generate CO with a high yield rate. The high stability and efficient electron transfer properties of Co9S8 cages make them promising for enhanced CO2 photoreduction performance.
Article
Chemistry, Organic
Haruki Mizoguchi, Ryuji Yoshida, Haruka Ikeda, Akira Sakakura
Summary: An intramolecular C-H silylmethylation of benzylic alcohol derivatives was achieved using a visible-light-photoexcited palladium complex as the catalyst. Blue LED irradiation activated a C-I bond, and subsequent intramolecular radical arylation led to the formation of siloxacycle products. Selective protonation or oxidation of the C-Si bond of the cyclized materials afforded ortho-methylated and ortho-hydroxymethylated derivatives of the benzylic alcohol derivatives.
Review
Chemistry, Multidisciplinary
Jiahao Wang, Xinxin Lv, Zhiyong Jiang
Summary: Asymmetric catalysis is a powerful tool for synthesizing enantioenriched molecules. Deracemization, the direct conversion of a racemic compound to one enantiomer, is an attractive approach with high-atom efficiency. Visible-light-driven photocatalysis has recently emerged as a promising platform for deracemization, overcoming kinetic and thermodynamic challenges in chemical transformations without the need for additional stoichiometric reagents. This review systematically summarizes and discusses the advances in this area, categorizing examples based on energy transfer and single-electron transfer in photocatalysis.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Christopher G. Bailey, Mitchell D. Nothling, Lucy L. Fillbrook, Yen Vo, Jonathon E. Beves, Dane R. McCamey, Martina H. Stenzel
Summary: Polydopamine (PDA) is a synthetic model for melanin and exhibits photo-responsive free radical properties under visible light. This discovery allows PDA to serve as a photo-redox catalyst and sensitizes exogenous species through photoinduced electron transfer. The utility of PDA nanoparticles as a photosensitizer is demonstrated by initiating free-radical polymerization of vinylic monomers. This study provides crucial insights into the photoactive free radical properties of melanin-like materials and highlights a promising application for PDA as a photosensitizer.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Cheol Hyeon Ka, Seoyeon Kim, Eun Jin Cho
Summary: Fluoroalkylation is an important synthetic process for modifying molecules with fluoroalkyl groups, which can enhance compound properties and have potential applications in medicine and materials science. The use of visible light-induced, metal-free methods is particularly important due to its environmental friendliness and elimination of potential risks associated with metal-catalyst toxicity. This Account describes our studies on visible light-induced, metal-free fluoroalkylation processes, using organic photocatalysts or EDA complexes. Various pi-systems have been successfully fluoroalkylated under the developed reaction conditions.
Article
Chemistry, Physical
Kai Sun, Masato Ueno, Keisuke Imaeda, Kosei Ueno, Masaya Sawamura, Yohei Shimizu
Summary: A boron-catalyzed alpha-allylation of carboxylic acids with allylsulfones under blue LED irradiation conditions has been developed. The photoexcitation of catalytically generated boron enediolates induces single-electron transfer to the allylsulfones, leading to subsequent C-C bond formation and the construction of sterically demanding quaternary carbon centers at the position a to the carboxy group. The p-extended ligand on the boron atom is likely crucial for the efficient photoexcitation of the boron enediolates.
Article
Chemistry, Multidisciplinary
Thomas J. J. Barnes, Jack Payne, Sebastian D. D. Pike
Summary: Cu-16-Cu-31 Cu(ii)-oxo-carboxylate clusters, including those with condensed 1.5 nm Cu-O cores supported exclusively by O-donor ligands, are reported. A size-colour correlation is observed with a red-shift in the charge transfer absorption band as the size increases, placing these clusters between small molecules and (black) CuO nanostructures.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Zhoushilin Ruan, Shenlong Jiang, Qun Zhang, Yi Luo
Summary: This study presents a systematic demonstration of phononic fine-tuning in a two-dimensional lead-halide perovskite system through fluorination. The effects of fluorination on the structural distortion-induced phononic properties are investigated using ultrafast spectroscopy and temperature-dependent photoluminescence spectroscopy. The results reveal the subtle but profound impacts of fluorination on coherent phonon modes, phonon-phonon/electron-phonon interactions, and the hot-phonon bottleneck effect.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Biochemistry & Molecular Biology
Wenjiang Zhaxi, Miao Li, Jing Wu, Luying Liu, Zetao Huang, Huixian Miao, Xiao Ma, Shenlong Jiang, Qun Zhang, Wei Huang, Dayu Wu
Summary: Solid-state lighting technology, using light-emitting diodes (LEDs) for energy conversion, is a next-generation lighting technology. This study reports the synthesis of high-efficiency phosphors for high flux white LED designs and analyzes their structure and photophysical properties. The results demonstrate that the synthesized phosphors exhibit excellent performance under high operating currents.
Article
Chemistry, Multidisciplinary
Congmin Zhang, Lichen Bai, Min Chen, Xuejiao Sun, Mengzhao Zhu, Qinglong Wu, Xiaoping Gao, Qun Zhang, Xusheng Zheng, Zhen-Qiang Yu, Yuen Wu
Summary: The site density of Mo single atoms on RPCN is controlled by a local carbonization strategy, capturing adventitious O atoms and forming O-covered Mo-N-3 coordination. Coordinated O atoms create a catalytic environment with Lewis base and gather photo-generated electrons under light. The resulting Mo-RPCN exhibits a strong ability for hydrogen abstraction.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Huixian Miao, Yujie Zhou, Pingping Wang, Zetao Huang, Wenjiang Zhaxi, Luying Liu, Fengnan Duan, Jinmin Wang, Xiao Ma, Shenlong Jiang, Wei Huang, Qun Zhang, Dayu Wu
Summary: In this study, the high-temperature negative thermal quenching (NTQ) effect was observed in copper iodide cluster-based coordination polymers that emit deep-red to near-infrared (NIR) light. The NTQ operating temperature of these unconventional phosphors can reach as high as 500 K, which is the highest temperature achieved by NTQ molecular-based materials.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Rui Mao, Dan Wu, Qun Zhang, Yang Chen
Summary: The ultraviolet photodissociation dynamics of 2-bromohexane around 234 nm was studied using the DC slice velocity map imaging technique. The relative quantum yield of the ground state bromine atom was measured to be 0.961. Analysis of the slice images revealed the speed and angular distributions of the ground state and excited state bromine atoms. The speed distribution consisted of two Gaussian components, attributed to two dissociation channels. The high translational energy component involved direct dissociation along the C-Br bond, while the low translational energy component involved multidimensional dissociation along the C-Br bond coupling with bending modes. The branching of alkyl radicals promoted the multidimensional dissociation. Furthermore, the contribution of the electric-dipole allowed 3Q1, 3Q0, and 1Q1 states to product formation was discussed, and the nonadiabatic 1Q1 <- 3Q0 transition played a significant role in the dissociation process.
Article
Chemistry, Multidisciplinary
Zhifeng Jiang, Zhiquan Zhang, Jianli Liang, Min Zhou, Daobin Liu, Danjun Mao, Qun Zhang, Wei Zhang, Huaming Li, Li Song, Taicheng An, Po Keung Wong, Chun-Sing Lee
Summary: An efficient catalyst is developed for CO2-to-CO conversion using diverse N-C-b materials with hierarchical pore structures. The surface local electric field originating from charge separation can be boosted by hierarchical pore structures, doped N, as well as pyridinic-N, thereby enhancing the CO2RR performance. These findings provide new insights into CO2RR on N-C-b and will guide the design of nature-based photocatalysts.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Renli Chen, Shenlong Jiang, Qun Zhang
Summary: In this study, we performed an experimental investigation on the intermolecular singlet fission (xSF) in the solution phase of a radical dianion system of PTCDA(2-). Our ultrafast spectroscopic results provide a comprehensive understanding of the elementary steps involved in the xSF process of photoexcited PTCDA(2-). Our findings demonstrate the applicability of the three-step model, typically used to describe crystalline-phase xSF, in the description of solution-phase xSF and the extension of xSF materials to charged radical systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Zhoushilin Ruan, Shenlong Jiang, Qun Zhang
Summary: Organic-cation engineering has been effective in regulating two-dimensional hybrid organic-inorganic perovskites (2D HOIPs) for various applications. The impact of organic cation modification on phonon dynamics, exciton dynamics, and excitonic emissions in this system is investigated. The findings provide valuable mechanistic insights for the applications of 2D HOIPs.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Xiancheng Pan, Shenlong Jiang, Qun Zhang, Yi Luo
Summary: We present the real-time tracking of explosive boiling dynamics at the alcohol/MXene interface by observing the photoinduced lattice dynamics of MXene nanosheets dispersed in different alcohols. The explosive boiling process is shown to undergo three cascading stages: starting initiation, phase explosion, and eventual termination. Photothermal modeling further reveals the conditions for explosive boiling, which align well with experimental observations, suggesting a phase transition from liquid to vapor in approximately 17-25 layers of alcohol molecules. This study provides valuable insights into thermal conduction/diffusion and transient acoustic pressure associated with the early stage of explosive boiling, enriching our fundamental understanding of this dynamic process at the liquid-solid interface.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Qun Zhang, Jun Bao, Jiawei Xue, Shenlong Jiang, Zhiyu Wang, Zhiyong Jiang, Heng Cao, Xiaodi Zhu, Yi Luo
Summary: Metal halide perovskites (MHPs) have attracted significant attention as catalysts in heterogeneous photocatalysis, due to their superior optoelectronic properties. Efficient dissociation of excitons into charge carriers is crucial for enhancing the photocatalytic performance of MHP-based catalysts. However, achieving efficient exciton dissociation has been challenging. In this study, we propose a novel concept of utilizing the edge interfacial state to trigger anisotropic electron transfer and promote exciton dissociation. We demonstrate the effectiveness of this concept by constructing a Cs4PbBr6/TiO2 mesocrystal heterojunction, which shows excellent performance in photocatalytic CO2 reduction. This work provides valuable insights for the rational design of advanced photocatalysts.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Letter
Chemistry, Multidisciplinary
Jun-Nan Yang, Zhen-Yu Ma, Jin-Da Luo, Jing-Jing Wang, Chunyin Ye, Yujie Zhou, Yi-Chen Yin, Xue-Chen Ru, Tian Chen, Lian-Yue Li, Li-Zhe Feng, Kuang-Hui Song, Jing Ge, Qun Zhang, Hong-Bin Yao
Summary: We report a resurfacing strategy using pseudohalogen ions to stabilize lead halide perovskite nanocrystal light-emitting diodes (PNC LEDs) by mitigating halide ion migration. By employing a thiocyanate solution processed post-treatment method, we successfully resurfaced CsPbBr3 nanocrystals and demonstrated that thiocyanate ions can effectively inhibit bromide ion migration in lead halide perovskite nanocrystal thin films. As a result of thiocyanate resurfacing, we achieved PNC LEDs with a high EQE of 17.3%, a maximum brightness of 48000 cd m(-2), and an excellent operation half-life time.
Article
Chemistry, Physical
Xiao-Hong Li, Hui Li, Shen-Long Jiang, Lan Yang, Hui-Yi Li, Qi-Long Liu, Wei Bai, Qun Zhang, Chong Xiao, Yi Xie
Summary: The strategy of constructing a mimic-enzyme catalyst for photocatalytic N-2 fixation based on MOFs and POMs can efficiently simulate the pi-backbonding mechanism of nitrogenase, leading to an efficient artificial conversion of N-2 to NH3 under mild conditions.
Article
Chemistry, Multidisciplinary
Qing Yao, Hui Li, Jiawei Xue, Shenlong Jiang, Qun Zhang, Jun Bao
Summary: Inspired by the success in the photovoltaic field, methylammonium lead iodide perovskite (MAPbI(3)) is explored as photocatalysts in H-2 evolution reactions. The distribution of defective areas is regulated to promote charge-transfer dynamics and achieve an impressive H-2 evolution rate. This work establishes a new paradigm for controlling charge-transfer dynamics in photocatalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Hui Li, Jiachen Zhang, Qun Zhang
Summary: Prolonging the lifetime of hot carriers in lead-halide perovskite quantum dots is desired for improving photovoltaic conversion efficiency. In this study, a new scenario of ligand engineering was proposed, featuring selective capping on the surface of CsPbBr3 QDs. Through various observations, it was revealed that phononic regulation of Pb-Br stretching at the Br-site effectively retards the hot-carrier cooling process, providing a new route for manipulating hot-carrier dynamics in perovskite systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Feifei Qiu, Zu-Yong Gong, Dongwei Cao, Ce Song, Guangjun Tian, Sai Duan, Yi Luo
Summary: Tip-enhanced fluorescence excitation (TEFE) is a new technique that utilizes highly confined plasmonic field to directly visualize the vibronic effect of a single molecule in real space for arbitrary excited states. Numerical simulations confirm that TEFE can identify vibronic couplings originating from Herzberg-Teller active modes.
