Article
Chemistry, Organic
Pietro Franceschi, Elena Rossin, Giulio Goti, Angelo Scopano, Alberto Vega-Penaloza, Mirco Natali, Deepak Singh, Andrea Sartorel, Luca Dell'Amico
Summary: In this study, we developed a novel photocarboxylation method using an organic photoredox catalyst and different dihydropyridine compounds in combination with an organic base. Through mechanistic investigations, we discovered the key role of a hydrogen bonding complex between the dihydropyridine and the base. This method allowed for the synthesis of carboxylic acids under mild reaction conditions, with good yields and synthetic versatility.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Yang Liu, Chensi Tang, Min Cheng, Ming Chen, Sha Chen, Lei Lei, Yashi Chen, Huan Yi, Yukui Fu, Ling Li
Summary: POM@MOF composites have been attracting attention in photocatalysis due to their enhanced performance, which benefits from the high specific surface area and long-range ordered structure of MOFs that ensure a uniform distribution of POMs and provide more active catalytic sites.
Review
Chemistry, Physical
Songying Qu, Hao Wu, Yun Hau Ng
Summary: Hydrogen peroxide is a crucial chemical attracting attention for energy and environmental applications. The environmentally friendly solar-driven production of hydrogen peroxide, which only requires water, oxygen, and light energy, has gained the most attention. The rational design of functional photo-responsive catalysts promotes hydrogen peroxide production in photo(electro)catalytic approaches. This review systematically summarizes strategies for these catalysts and discusses prevailing hypotheses, state-of-the-art catalysts, critical challenges, and perspectives to enhance comprehension and promote interest in sustainable hydrogen peroxide production.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Lei Zou, Rongjian Sa, Hong Zhong, Haowei Lv, Xinchen Wang, Ruihu Wang
Summary: In this study, a CdS@COF core-shell structure was successfully synthesized through a structural and electronic engineering strategy, which significantly improved the efficiency of photocatalytic CO2 reduction. The integration of CdS as an electron transfer channel enables photoelectron transfer and subsequent CO2 reduction from Zn-porphyrin to Co-bipyridyl units.
Article
Energy & Fuels
Huaxing Lin, Chunping Chen, Tianhua Zhou, Jian Zhang
Summary: Covalent organic frameworks (COFs) are crystalline porous materials with organic building blocks linked by covalent bonds, and 2D COFs have emerged as promising photocatalysts with extended π-conjugated skeletons, high surface area, and high crystallinity.
Review
Chemistry, Multidisciplinary
Hailing Huo, Fang Wu, Erjun Kan, Ang Li
Summary: The overall photocatalytic CO2 reduction reaction (PCRR) is crucial for CO2 utilization and solar energy conversion. However, efficient conversion remains a challenge. This Review summarizes strategies developed in the past decade, such as self-driving material development, Z-scheme heterojunction construction, cocatalyst loading, heteroatom doping, surface vacancy creation, and carrier-material matching. The future research directions in this field are also discussed.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Nanoscience & Nanotechnology
Shangcong Sun, Bo Peng, Ye Song, Ruoyu Wang, Haitao Song, Wei Lin
Summary: In this study, a Z-scheme iron oxyhydroxide/ polymeric carbon nitride (FeOOH/PCN) heterojunction was constructed to overcome the challenges of sluggish water oxidation kinetics and severe charge recombination in solar-driven conversion of carbon dioxide. The FeOOH nanorod provided abundant coordinatively unsaturated sites and oxidative photoinduced holes, enhancing the water decomposition kinetics. PCN acted as a stable agent for CO2 reduction. As a result, FeOOH/PCN achieved efficient CO2 photoreduction with a high selectivity of CH4 (>85%) and an apparent quantum efficiency of 2.4% at 420 nm, surpassing most two-step photosystems to date. This work introduces an innovative strategy for the construction of photocatalytic systems for solar fuel production.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Environmental
Chuang Yang, Ji-Ming Yu, Longfei Zhai, Shanqing Jia, Ting Yang, Wei-Wei Xiong, Qichun Zhang
Summary: In order to efficiently reduce Cr(VI) through photocatalysis, researchers have developed an organic hybrid selenidostannate [Ni(phen)(3)][Sn3Se7]center dot 1.5H(2)O (NPTS) coupled with polyaniline (PANI) to form NPTS@PANI-x (x = 15, 50, 100) composites. These composites exhibit excellent photocatalytic performance in reducing Cr(VI), with NPTS@PANI-15 capable of reducing 100% of Cr(VI) (100 mg/L) in 10 minutes. The research demonstrates the potential of organic hybrid metal chalcogenides as highly efficient photocatalysts for Cr(VI) reduction.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
J. Andrew P. Maitland, Jamie A. Leitch, Ken Yamazaki, Kirsten E. Christensen, Doyle J. Cassar, Trevor A. Hamlin, Darren J. Dixon
Summary: This study describes a reagent-controlled stereodivergent carbocyclisation of aryl aldimine-derived, photocatalytically generated alpha-amino radicals possessing adjacent conjugated alkenes. The reaction can afford either bicyclic or tetracyclic products, with high selectivity and good-to-excellent yields. Computational analysis using DFT revealed the reaction pathway and mechanistic rationale behind this finely balanced yet readily controlled photocatalytic system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Energy & Fuels
Nikolaos Karamoschos, Dimitrios Tasis
Summary: Hydrogen peroxide (H2O2) has a wide range of applications, and the photocatalytic synthesis of H2O2 is a green alternative strategy that utilizes renewable energy sources. This review discusses the milestones achieved in the development of functional photocatalytic systems, exploring different semiconductors and surface dopants to improve H2O2 production rates and inhibit degradation.
Article
Chemistry, Multidisciplinary
Hanning Li, Yang Yang, Xu Jing, Cheng He, Chunying Duan
Summary: This study demonstrates that incorporating multiple photoactive units into metal-organic frameworks can enhance the photocatalytic activity for hydrogen production and organic oxidation, and the multi-component strategy can effectively promote the efficient charge separation and excellent photocatalytic activity of the catalyst.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Review
Chemistry, Multidisciplinary
Yang Wang, Yong Yang, Qinghua Deng, Weibing Chen, Yongcai Zhang, Yong Zhou, Zhigang Zou
Summary: The establishment of green and environmental friendly sunlight-driven organic reactions has gained attention since the 21st century. Porous organic polymers (POPs) have shown great promise in photocatalytic organic reactions due to their functional designability, micromesoporous structure, and thermal/chemical stability. This review focuses on various amorphous POP materials and synthetic strategies, as well as the research progress in photocatalytic oxidation, coupling, reduction, cycloaddition, and polymerization reactions. The challenges and prospects for future research on amorphous POPs are also discussed.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Environmental Sciences
Yaru Wang, Yechen Wang, Xubo Huang, Min Chen, Yiming Xu
Summary: This study reports an improved activity of Bi2MoO6 (BMO) through the addition of nickel hexammine perchlorate (NiNH). NiNH greatly increased the rate of phenol oxidation on BMO and facilitated the charge separation of BMO.
JOURNAL OF ENVIRONMENTAL SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Qian Liu, Shihong Wang, Weihao Mo, Yiyi Zheng, Yanbo Xu, Guodong Yang, Shuxian Zhong, Jun Ma, Dong Liu, Song Bai
Summary: The study demonstrates a strategy for spatial separation of redox cocatalysts on various semiconductors through a unique stacked photocatalyst design, showing superior activity and stability. This smart design helps mitigate charge recombination, provide highly active and selective sites, and protect semiconductors from photocorrosion.
Article
Chemistry, Physical
Yaru Wang, Jianjun Zhao, Min Chen, Xubo Huang, Yiming Xu
Summary: The co-deposition of Pt and nickel phosphate (NiP) as co-catalysts can accelerate the degradation of organic compounds and improve the efficiency of semiconductor photocatalysis. This method not only promotes electron and hole transfer but also enhances the efficiency of charge separation, leading to increased rates of surface reactions.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Engineering, Biomedical
Kangqiang Qiu, Ryo Seino, Guanqun Han, Munetaka Ishiyama, Yuichiro Ueno, Zhiqi Tian, Yujie Sun, Jiajie Diao
Summary: Endocytosis is a crucial cellular process for taking up nutrients and maintaining cellular homeostasis. Using the membrane-anchored pH probe ECGreen and structured illumination microscopy (SIM), the dynamics of endocytic vesicles can be visualized and analyzed. The multidimensional analysis model developed using ECGreen provides spatial, temporal, and pH information, allowing for a better understanding of endocytosis.
ADVANCED HEALTHCARE MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Chuang Han, Guanqun Han, Shukai Yao, Lan Yuan, Xingwu Liu, Zhi Cao, Arun Mannodi-Kanakkithodi, Yujie Sun
Summary: This study introduces a noble metal-free and ultrathin ZnIn2S4 photocatalyst for deuteration reactions using heavy water as the sole deuterium source. By synthesizing defective two-dimensional ZIS nanosheets with surfactant assistance, the performance is significantly enhanced.
Article
Chemistry, Multidisciplinary
Bidyut Kumar Kundu, Guanqun Han, Yujie Sun
Summary: In this study, two novel two-photon-absorbing organic photosensitizers were reported, which can be driven by NIR light irradiation using inexpensive LED as the light source. By modulating the donor-pi-acceptor-pi-donor conjugated structure, excellent two-photon absorption capability in the NIR region was achieved. These organic photosensitizers exhibited superior performance in driving various O2-involved organic reactions under 850 nm light irradiation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Guodong Li, Guanqun Han, Lu Wang, Xiaoyu Cui, Nicole K. Moehring, Piran R. Kidambi, De-en Jiang, Yujie Sun
Summary: This study reports a new method for water electrolysis hydrogen production using a Cu3Ag7 electrocatalyst to replace the sluggish oxygen evolution reaction with the more favorable partial oxidation of formaldehyde to formate under alkaline conditions. The strategy not only produces more valuable anodic product than O-2 but also releases H-2 at the anode with a small voltage input.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Hui Jiang, Yujie Sun, Bo You
Summary: Closed-loop cycling of green hydrogen, stored from renewable energy sources, is a promising alternative for mitigating the energy crisis and environmental pollution. However, the sluggish kinetics of involved reactions and the need for rapid mass transport and gas diffusion pose challenges. This Account summarizes the contributions of dynamic electrodeposition on bubbles to the development of advanced porous electrocatalysts for green hydrogen cycling.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Chuang Han, Guanqun Han, Md Habibur Rahman, Arun Mannodi-Kanakkithodi, Yujie Sun
Summary: Visible-light-driven C-C bond formation utilizing ketyl radical (C-ketyl) species has attracted attention due to its direct synthesis route for complex molecules. However, current photocatalytic systems suffer from high cost and potential degradation, making product separation and purification challenging. This study demonstrates the use of readily accessible and inexpensive semiconductor ZnIn2S4 for efficient synthesis of industrially important chemicals through intramolecular cyclization and intermolecular cross-coupling reactions using ketyl radicals. Experimental and computational investigations provide mechanistic insights for these reactions on ZnIn2S4.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Kaili Yan, Hyuna Kwon, Morgan Huddleston, De-en Jiang, Yujie Sun
Summary: Electrocatalytic biomass valorization has gained increasing interest, but reports on pyridine-containing chemicals from biomass upgrading are rare. In this study, we describe an electrochemical synthesis of 3-pyridinol from biomass-derived furfurylamine, achieving a 97% yield. The use of a Br-/Br+ redox cycle and strong acidic conditions was crucial for driving the final dehydration step. Control experiments and computational investigations were conducted to elucidate the key mechanistic steps of the one-pot conversion of furfurylamine to 3-pyridinol.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Bidyut Kumar Kundu, Chuang Han, Prasenjit Srivastava, Siddhant Nagar, Katie E. E. White, Jeanette A. A. Krause, Christopher G. G. Elles, Yujie Sun
Summary: A metal-free organic photocatalyst, dBIP-OMe, was reported for the photocatalytic trifluoromethylation of alkenes without the use of sacrificial reagents. Mechanistic studies revealed two consecutive single-electron-transfer reactions between dBIP-OMe, CF3 precursor, and the alkene substrate. The trifluoromethylative bifunctionalization strategy using dBIP-OMe was applicable for both aryl and aliphatic alkenes, and various nucleophiles could be easily incorporated into the carbocation intermediate, broadening the application scope of this photocatalytic method.
Article
Chemistry, Multidisciplinary
Rui Chen, Lei Wang, Guodong Ding, Guanqun Han, Kangqiang Qiu, Yujie Sun, Jiajie Diao
Summary: Endolysosome dynamics is crucial for autophagosome biogenesis. A cationic quinolinium-based fluorescent probe (PyQPMe) with pH-sensitive fluorescence in endolysosomes is reported here, enabling high-resolution imaging and deepening understanding of autophagy. The probe's large Stokes shift and strong fluorescence intensity reduce background noise, providing a high signal-to-noise ratio for imaging. Application of PyQPMe revealed a constant conversion rate from early to late endosomes/lysosomes during autophagy at the submicron level.
Article
Chemistry, Physical
Guanqun Han, Guodong Li, Yujie Sun
Summary: The use of palladium membrane electrodes allows for electrocatalytic dual hydrogenation of unsaturated dicarboxylic acids by physically separating the formation of hydrogen from the hydrogenation reaction. This design enables the simultaneous hydrogenation of the same substrate at both the anode and cathode, achieving a theoretical maximum Faradaic efficiency of 200%.
Review
Chemistry, Multidisciplinary
Chuang Han, Bidyut Kumar Kundu, Yujun Liang, Yujie Sun
Summary: This review article provides an overview of recent advancements in utilizing near-infrared (NIR) light for photocatalysis, with a particular focus on the emerging field of two-photon excitation NIR photocatalysis. The article highlights the advantages of utilizing NIR light and two-photon excitation compared to UV-visible irradiation and one-photon excitation.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Md. Habibur Rahman, Jiaqi Yang, Yujie Sun, Arun Mannodi-Kanakkithodi
Summary: ZnIn2S4 has attracted research interest as a semiconductor-based chalcogenide photocatalyst due to its visible light absorption, stability, and low cost. However, its photocatalytic activity is affected by limited visible light absorption and fast recombination of photogenerated charge carriers. In this study, defect energetics in ZnIn2X4 compounds were investigated using density functional theory (DFT), providing valuable insights for experimental design and defect engineering.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Rui Chen, Kangqiang Qiu, Guanqun Han, Bidyut Kumar Kundu, Guodong Ding, Yujie Sun, Jiajie Diao
Summary: Using the fluorescent probe PCV-1 under super-resolution microscopy, this study visualized cell viability and developed an analytical assay called organelle ratiometric probing (ORP) for quantitative analysis and assessment of individual cell viability. This method is of great significance in gaining deeper insights into the mechanisms of cell death.
Article
Chemistry, Multidisciplinary
Rui Chen, Kangqiang Qiu, Guanqun Han, Bidyut Kumar Kundu, Guodong Ding, Yujie Sun, Jiajie Diao
Summary: Detecting cell viability at the single-cell level is crucial in cancer research. We have developed a fluorescent probe, PCV-1, which can visualize cell viability under super-resolution imaging. By comparing the fluorescence intensity of mitochondria and nucleoli, we have developed an analytical assay named ORP to quantitatively analyze and assess cell viability at the single-cell level.
Article
Chemistry, Multidisciplinary
Kaili Yan, Morgan L. Huddleston, Brett A. Gerdes, Yujie Sun
Summary: Electrochemical conversion of biomass-derived intermediate compounds to high-value products is a promising approach in biorefinery, with relatively little attention given to amino acids as products. This study reports an electrochemical approach that combines selective oxidation and electrochemical reductive amination for efficient production of amino acids.
