Article
Chemistry, Multidisciplinary
Daniela Cappello, Francis L. Buguis, Joe B. Gilroy
Summary: Molecular materials with pi-conjugated donor-acceptor and acceptor-donor-acceptor structures have versatile applications in organic photovoltaic materials, organic light-emitting diodes, and biological imaging agents. Boron-containing compounds with unique optoelectronic and redox properties are synthesized using Stille cross-coupling chemistry. The compounds exhibit reversible redox waves, solid-state emission, and aggregation-induced emission. The optical band gaps determined from experiments and density functional theory calculations support the rationalization of the observed optoelectronic properties. This study provides a foundation for incorporating these boron-containing compounds into applications that require fine-tuning of band gaps.
Article
Chemistry, Multidisciplinary
Svenja Neumann, Oliver S. Wenger, Christoph Kerzig
Summary: The study investigates a molecular dyad capable of producing reduced metal complexes through an indirect pathway, demonstrating the potential of novel photocatalysts with unprecedented quantum yields. By optimizing this approach, the generation of reduced metal complexes via this pathway could outperform the conventional direct metal complex photoreduction. This research provides valuable evidence for the indirect mechanism of reduced metal complex generation and its advantages over direct pathways.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Chengxi Li, Xue Jin, Jianlei Han, Tonghan Zhao, Pengfei Duan
Summary: This article discusses the circularly polarized luminescence (CPL) activity of chiroptical materials, emphasizing the importance of increasing the dissymmetry factor glum value. Recent studies have shown that amplification of glum value can be achieved in hybrid donor-acceptor systems, providing new insights for the development of highly efficient CPL materials.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Review
Chemistry, Inorganic & Nuclear
Carolin Mueller, Sebastian Bold, Murielle Chavarot-Kerlidou, Benjamin Dietzek-Ivansic
Summary: In recent years, dyads in which molecular donor and acceptor moieties are chemically linked by a bridging ligand have shown promise in light-driven catalysis. The modular structure, control-lable donor-acceptor distance, and light-driven charge transfer abilities make these systems attractive for light-driven charge-transfer reactions and light-driven redox catalysis. This review discusses the role of 1,2,3-triazole bridging motif in driving electron transfer in triazole-bridged donor-acceptor dyads upon photoexcitation, and how the structural and electronic properties of the bridge influence charge separation and recombination rates. Criteria for designing dyads with different electron transfer properties are also derived.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Medicinal
Jiafeng Li, Aiyan Ji, Meiling Lei, Liwen Xuan, Ruihu Song, Xin Feng, Haixia Lin, Hao Chen
Summary: Nowadays, the development focus of NIR-II dyes is on achieving longer absorption/emission wavelength and higher quantum yield. However, this often leads to larger molecular weight and poor druggability due to the extended pi conjugation system. In this study, a reduced pi conjugation system D-A probe (TQ-1006) was synthesized, showing comparable excellent imaging performance and a higher T/N ratio compared to its D-A-D counterpart (TQT-1048). A conjugated probe (TQ-RGD) demonstrated extra high contrast tumor imaging, further proving the excellent NIR-II biomedical imaging applications of D-A dyes. Overall, the D-A framework offers a promising approach for designing next-generation NIR-II fluorophores.
JOURNAL OF MEDICINAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Shengfei Jin, Xianwei Sui, Graham C. Haug, Viet D. Nguyen, Hang T. Dang, Hadi D. Arman, Oleg Larionov
Summary: Progress in developing photocatalytic reactions requires a detailed understanding of the underlying mechanisms, especially those involving electron donor-acceptor complexes. This study reports a new method for regioselective installation of two different acyl groups through photocatalytic alkene 1,2-diacylation. The research highlights the central role of electron donor-acceptor complexes in mediating the photoinduced charge transfer process and sheds light on the catalytic activities of N-heterocyclic carbenes in radical reactions.
Article
Chemistry, Physical
Courtney A. DelPo, Saeed-Uz-Zaman Khan, Kyu Hyung Park, Bryan Kudisch, Barry P. Rand, Gregory D. Scholes
Summary: Enhanced delocalization is beneficial for absorbing molecules in organic solar cells, and polaritons offer exceptional delocalization that can improve the efficiency of bilayer organic photovoltaics by aiding in exciton delivery to the donor-acceptor interface. The decay of polaritons in bilayer cavities shows an additional pathway through charge transfer, indicating that the charge transfer from the polariton is fast enough to outcompete decay to the ground state.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Puja Agarwala, Enrique D. Gomez, Scott T. Milner
Summary: This study presents a coarse-graining method for simulating conjugated polymers, allowing for faster and more accurate investigation of their structure and properties. The method is validated through simulations of donor and acceptor polymers, which reveal the influence of interface width and slow cooling on polymer morphology.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Xingwang Lan, Xiaopeng Liu, Yize Zhang, Qing Li, Juan Wang, Qianfan Zhang, Guoyi Bai
Summary: The acetylene-bridged CTFs, featuring extended donor-π-acceptor motifs, demonstrated higher photocatalytic activity and achieved a higher apparent quantum efficiency in metal-free oxidative amines coupling reaction under visible-light irradiation. The acetylene moieties also provide active sites to enhance photoredox catalysis, showing the potential for high-performance CTFs in solar-to-chemical energy conversion.
Article
Chemistry, Physical
Thomas P. P. Fay, David T. T. Limmer
Summary: In this paper, a physically motivated framework is proposed to describe spin-selective recombination processes in chiral systems. Spin-selective reaction operators for recombination reactions of donor-bridge-acceptor molecules are derived based on chirality and spin-orbit coupling. It is found that spin polarization selectivity only arises in hopping-mediated electron transfer. The framework presented here can be extended to describe spin-selective recombination processes in more complex systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Engineering, Environmental
Yu Luo, Yuanfang Lin, Zonglin Weng, Bin Han, Yang Zhou, Xinwen Ou, Jin Jiang
Summary: By grafting thiophene (TP) onto the edge of g-C3N4, a donor-acceptor-engineered catalyst (g-C3N4-TP) is developed for efficient H2O2 production. The optimized g-C3N4-TP exhibits a significantly enhanced H2O2 production rate compared to pristine g-C3N4, attributed to the introduced TP units that promote electron-hole separation, alter O2 adsorption mode, and reduce energy barriers for H2O2 production. This work provides insights into O2 adsorption and conversion on g-C3N4 and suggests a new approach for efficient H2O2 production via rational design of donor-acceptor-engineered photocatalysts.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Wei He, Jing Zhou, Wenhua Xu, Chengbo Li, Jun Li, Ning Wang
Summary: This study investigates the effect of donor unit content on the photoelectric properties and photocatalytic activity of covalent triazine frameworks (CTFs). It is found that increasing the donor unit content can improve photocatalytic activity, attributed to stronger visible light absorption capacity and higher charge carrier separation efficiency.
Article
Chemistry, Applied
Yoliztli Banales-Leal, Andrea Garcia-Rodriguez, Fabian Cuetara-Guadarrama, Mireille Vonlanthen, Kendra Sorroza-Martinez, David Morales-Morales, Ernesto Rivera
Summary: A novel series of dendritic compounds with peripheral pyrene groups and a porphyrin core were synthesized and characterized in this study. Metallation with Zn(II) and Mg(II) resulted in red shifts in the Soret absorption band and blue shifts in the emission band for the dendritic porphyrins, with all compounds exhibiting high energy transfer efficiency.
Article
Chemistry, Applied
Fang-Zhou Li, Xing-Yu Li, Wenjun Ni, Zhi-Wei Wu, Changwei Lin, Gagik G. Gurzadyan, Gui-Chao Kuang
Summary: By finely tuning various parameters, the novel donor-acceptor-donor (D-A-D') type of BODIPY derivative BDP-1 exhibited single component white light emission (WLE), achieved through the balance between aggregation and energy transfer (ET) and intramolecular charge transfer (CT).
Review
Chemistry, Applied
Barakha Saxena, Roshan I. I. Patel, Anuj Sharma
Summary: Quaternary pyridinium compounds are widely used intermediates in organic synthesis and have gained popularity in the field. Traditional methods for transforming these compounds into C-C and C-X bonds require high temperatures, expensive catalysts, and specific conditions. However, researchers have sought alternative strategies that do not rely on transition metal or photocatalysis. Electron-donor-acceptor (EDA) complex reactions have emerged as an effective method, utilizing the electron-acceptor ability of quaternary pyridinium derivatives to generate radical intermediates without the need for photocatalysts. This review discusses the progress, mechanism, substrate scope, and limitations of EDA-complex mediated reactions involving quaternary pyridinium compounds.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Zhicheng Jin, Yi Li, Ke Li, Jiajing Zhou, Justin Yeung, Chuxuan Ling, Wonjun Yim, Tengyu He, Yong Cheng, Ming Xu, Matthew N. Creyer, Yu-Ci Chang, Pavla Fajtova, Maurice Retout, Baiyan Qi, Shuzhou Li, Anthony J. O'Donoghue, Jesse V. Jokerst
Summary: In this study, a colorimetric biosensor using plasmonic gold and surfactant-like peptides (SLPs) was developed, which exhibited a strong aggregation propensity of the FFPC tail without the polar DDD head. The SLPs had specificity towards the target protease M-pro, a biomarker for SARS-CoV-2. This simple and visual tool showed detection limits of 15.7, 20.8, and 26.1 nM for M-pro in phosphate buffer, exhaled breath condensate, and saliva, respectively, and may have potential in designing other protease testing methods.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Haoyang Fu, Jiaqi Wei, Guoliang Chen, Minkai Xu, Jiyuan Liu, Jianghong Zhang, Ke Li, Qianyu Xu, Yunjie Zou, Wei-xian Zhang, Shibo Xi, Xiaodong Chen, Shuzhou Li, Lan Ling
Summary: This study reports a strategy to regulate the coordination status of single-atom catalysts (SACs) by introducing iron phthalocyanine on N-doped graphene to achieve a Fenton-like SAC containing an axial five-coordinated configuration (Fe-N5). The Fe-N5 SAC significantly modulates the electronic state of Fe atoms and lowers the activation energy for the production of center dot OH. Additionally, it shortens the diffusion distance of center dot OH by establishing a dual-site reaction mechanism with enriched pyridinic N sites, resulting in exceptional Fenton activity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Materials Science, Multidisciplinary
Chun-Yu Cheng, Yuan-Yuan Guo, Yi-Ming Zou, Amanda Jiamin Ong, Alfred Iing Yoong Tok, Shuzhou Li
Summary: The melting mechanisms of Pt-based multimetallic nanoparticles (NPs) were investigated using molecular dynamics (MD) simulation. The study found that the melting and coalescence behaviors of heterogeneous Pd-Pt NPs with different sizes and compositions varied, and PtPd alloy could form at the Pd/Pt interface before complete melting of Pd NP. Furthermore, a two-step melting process was observed in Pd/Pt/Ir trimetallic NPs.
Article
Nanoscience & Nanotechnology
Bo Niu, Delong Cai, Zhihua Yang, Xiaoming Duan, Wenjiu Duan, Donghui Long, Shuzhou Li, Dechang Jia, Yu Zhou
Summary: The high-temperature dielectric loss of hexagonal boron nitride (h-BN) ceramics can be reduced by orienting grains, leading to a minimized defect ions transport and lower dielectric loss.
SCRIPTA MATERIALIA
(2023)
Article
Physics, Condensed Matter
Saeed Yazdani, Kourtney Collier, Grace Yang, Jared Phillips, Ashley Dale, Aaron Mosey, Samuel Grocki, Jian Zhang, Anne E. Shanahan, Ruihua Cheng, Peter A. Dowben
Summary: Using optical characterization, the study shows that the spin state of the spin crossover molecular complex [Fe{H2B(pz)(2)}(2)(bipy)] is influenced by the electric polarization of the adjacent polymer ferroelectric polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) thin film. The role of the PVDF-HFP thin film is significant but complex. UV-Vis spectroscopy measurements reveal that the electronic structure of [Fe{H2B(pz)(2)}(2)(bipy)] molecules in bilayers of PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] can switch as a function of ferroelectric polarization at room temperature. The retention of voltage-controlled nonvolatile changes to the electronic structure in bilayers of PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] strongly depends on the thickness of the PVDF-HFP layer. The PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] interface may affect PVDF-HFP ferroelectric polarization retention in the thin film limit.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Chemistry, Multidisciplinary
Yuchen Hu, Xin Zhang, Rebecca Shu Hui Khoo, Christian Fiankor, Xu Zhang, Jian Zhang
Summary: By reducing the size of the primary ligand, we synthesized NPF-320, a Zr-MOF with optimized pocket sizes. This MOF allows for the post-synthetic installation of three secondary linkers in all six permuted sequences, forming a quinary MTV-MOF. With the functionalization of these linkers, we can construct MTV-MOFs with variable porosity and unprecedented complexity and encoded synthetic sequence information.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Lingfei Tang, Bowen Chen, Zhonghan Zhang, Changqi Ma, Junchao Chen, Yage Huang, Fengrui Zhang, Qingyu Dong, Guoyong Xue, Daiqian Chen, Chenji Hu, Shuzhou Li, Zheng Liu, Yanbin Shen, Qi Chen, Liwei Chen
Summary: Solid polymer electrolytes (SPEs) are considered promising electrolyte for long-cycling lithium metal batteries (LMBs). However, the narrow electrochemical stability window (ESW) of typical SPEs limits the improvement of LMBs' specific capacity and energy density. In this study, a polyfluorinated crosslinker was applied to enhance the oxidation resistance of SPEs, resulting in a wide ESW and improved performance of high-voltage LMBs.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Yuanmiao Sun, Jiarui Wang, Shibo Xi, Jingjing Shen, Songzhu Luo, Jingjie Ge, Shengnan Sun, Yubo Chen, John V. Hanna, Shuzhou Li, Xin Wang, Zhichuan J. Xu
Summary: In this study, the relationship between surface reconstruction of spinel electrocatalysts and metal-oxygen covalency polarity was investigated. It was found that a stronger metal-oxygen covalency contributes to a more thorough surface reconstruction towards oxyhydroxides. The researchers also developed a criterion to evaluate the reconstruction degree and provide guidelines for cation selection in spinel pre-catalyst design.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Ceramics
Yuchen Liu, Yu Zhou, Dechang Jia, Zhihua Yang, Wenjiu Duan, Daxin Li, Shuzhou Li, Ralf Riedel, Bin Liu
Summary: Using ab-initio calculations, the atomic structure and mechanical properties of amorphous silicoboron carbonitride ceramics with 13 different compositions in the Si-BN-C phase diagram were investigated. The chemical bonds and local structures in the amorphous network are dependent on the elemental composition. The mechanical properties of SiBCN ceramics are greatly influenced by their local structural characteristics. SiB2C3N2 and SiB3C2N3 with low Si contents and moderate C and/or BN contents exhibit high elastic moduli, high tensile/shear strengths, and good debonding capability. The optimization of SiBCN ceramics can be guided based on these discoveries.
JOURNAL OF ADVANCED CERAMICS
(2023)
Article
Chemistry, Multidisciplinary
Chin Guan Ho, Magdiel I. Setyawati, Glen M. DeLoid, Ke Li, Sunil S. Adav, Shuzhou Li, Say Chye Joachim Loo, Philip Demokritou, Kee Woei Ng
Summary: Exploitation of nature-derived materials is important for environmental sustainability, and cellulose is particularly interesting due to its abundance. Cellulose nanofibers (CNFs) have found applications as emulsifiers and lipid digestion modulators in food. This report demonstrates that CNFs can be modified to modulate toxin bioavailability in the gastrointestinal tract by forming inclusion complexes and promoting interaction with surface hydroxyl groups. Functionalized CNFs (FCNFs) were shown to effectively interact with the pesticide boscalid, and using an in vitro GIT simulation platform, it was found that FCNFs had a greater effect in retarding triglyceride digestion and binding boscalid in a simulated intestinal fluid environment. Overall, FCNFs have the potential to be developed into a functional food ingredient for modulating food digestion and toxin uptake.
Article
Chemistry, Physical
Tian Chen Li, Congjian Lin, Min Luo, Pinji Wang, Dong-Sheng Li, Shuzhou Li, Jiang Zhou, Hui Ying Yang
Summary: An efficient adsorptive additive strategy is proposed to reshape the electric double layer and regulate Zn interfacial chemistry, solving the problem of unstable Zn interface caused by undesired dendrites and parasitic side reactions. The self-adaptive adlayer constructed creates a horizontally aligned Zn deposition along the (002) plane and a localized environment lacking H2O and SO4 (2-), resulting in thermodynamically stable and highly reversible Zn electrochemistry. The achieved reversible plating/stripping of 3800 h and high Coulombic efficiency of 99.8% demonstrate the potential for practical application in a scalable, low-cost, rechargeable battery.
ACS ENERGY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Ashley S. Dale, Saeed Yazdani, Thilini K. Ekanayaka, Esha Mishra, Yuchen Hu, Peter A. Dowben, John W. Freeland, Jian Zhang, Ruihua Cheng
Summary: In this work, clear evidence of magnetic anisotropy in the local orbital moment of a molecular thin film based on the SCO complex [Fe(H2B(pz)(2))(bipy)] (pz = pyrazol-1-yl, bipy = 2,2'-bipyridine) is provided. The magnetic easy axis for the orbital moment is found to be along the surface normal direction, indicating the presence of an anisotropic energy barrier in the high-spin state. The observed magnetocrystalline anisotropy is mostly due to spin-orbit coupling, with spin- and orbital-component anisotropies determined to be 30.9 and 5.04 meV molecule(-1), respectively. The g factor in the range of 2.2-2.45 is consistent with the expected values. This work paves the way for understanding the spin-state-switching mechanism in the presence of magnetic perturbations.
JOURNAL OF PHYSICS-MATERIALS
(2023)
Article
Chemistry, Physical
Siwen Zhao, Mingwei Chang, Jiyuan Liu, Guoshuai Shi, Yuqin Yang, Huoliang Gu, Jianghong Zhang, Chunlei Yang, Haonan Tong, Chenyuan Zhu, Kecheng Cao, Shuzhou Li, Liming Zhang
Summary: Mitigating nitrogen oxide emissions is crucial for addressing global warming and improving air quality. Electrochemically converting nitrogen oxide pollutants into valuable fuels such as ammonia and hydroxylamine is of great significance, but current methods are hindered by complex reaction pathways and slow kinetics. In this study, we demonstrated that monodispersed transition-metal sites, specifically iron and nickel, can efficiently electrocatalyze nitric oxide conversion with high selectivity, activity, and durability. The metal centers strongly regulate the distribution of nitrogen products, with nickel favoring ammonia production and iron exhibiting superior selectivity towards hydroxylamine. Operando Fourier transform infrared spectroscopy provided insights into the different NO adsorption capabilities of single-atomic nickel and iron, which explain the different reduction pathways observed.
Article
Materials Science, Multidisciplinary
Huiying Yao, Xing Huang, Shuzhou Li, Wei Xu, Jia Zhu
Summary: For electrocatalysts, the electrocatalytic activity of non-metal sites cannot be ignored. The sulfur atoms in benzenehexathiol (BHT) based conjugated metal-organic frameworks (c-MOFs) are found to be the predominant active sites for the hydrogen evolution reaction (HER). The HER activity shows a volcano-shaped relationship with the 3p band center of the sulfur active site. Interlayer interactions also play a crucial role in determining the HER activity of c-MOFs. Based on these findings, we propose that Mo-BHT has excellent potential as an active HER catalyst.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Applied
Qiuhua Liu, Junhao Gao, Qin Lin, Borong Liao, Qian Zhang, Zaichun Zhou
Summary: A 21-oxaporphyrin was synthesized and found to play a crucial role in stabilizing cuprous ion through the synergy of diameter expansion and univalent form of the N3O core.
APPLIED ORGANOMETALLIC CHEMISTRY
(2023)