Single-Atom Titanium on Mesoporous Nitrogen, Oxygen-Doped Carbon for Efficient Photo-thermal Catalytic CO2 Cycloaddition by a Radical Mechanism
Angew Chem Int Ed Engl. 2024 Apr 6:e202404911. doi: 10.1002/anie.202404911. Online ahead of print.ABSTRACTDeveloping efficient and earth-abundant catalysts for CO2 fixation to high value-added chemicals is meaningful but challenging. Styrene carbonate has great market value, but the cycloaddition of CO2 to styrene oxide is difficult due to the high steric hindrance and weak electron-withdrawing ability of the phenyl group. To utilize clean energy (such as optical energy) directly and effectively for CO2 value-added process, we introduce earth-abundant Ti single-atom into the mesoporous nitrogen, oxygen-doped carbon nanoshe...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Yifan Wang Huimin Liu Qiujin Shi Zerui Miao Haohong Duan Yiou Wang Hongpan Rong Jiatao Zhang Source Type: research
Elucidation of Palmarumycin Spirobisnaphthalene Biosynthesis Reveals a Set of Previously Unrecognized Oxidases and Reductases
In this study, we elucidated the biosynthesis of palmarumycins, using gene disruption, heterologous expression, and substrate feeding experiments. The biosynthetic gene cluster for palmarumycins was identified to be distant from the polyketide synthase gene cluster, and included two cytochrome P450s (PalA and PalB), and one short chain dehydrogenase/reductase (PalC) encoding genes as key structural genes. PalA is an unusual, multifunctional P450 that catalyzes the oxidative dimerization of 1,8-dihydroxynaphthalene to generate the spiroketal linkage and 2,3-epoxy group. Chemical synthesis of key intermediate and in vitro bi...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Siji Zhao Zhen Shen Ziqi Zhai Ruya Yin Dan Xu Mingan Wang Qi Wang You-Liang Peng Ligang Zhou Daowan Lai Source Type: research
Covalent Organic Framework Interlayer Spacings as Perfectly Selective Artificial Proton Channels
Angew Chem Int Ed Engl. 2024 Apr 6:e202402094. doi: 10.1002/anie.202402094. Online ahead of print.ABSTRACTBiological proton channels have perfect selectivity in aqueous environment against almost all ions and molecules, a property that differs itself from other biological channels and a feature that remains challenging to realize for bulk artificial materials. The biological perfect selectivity originates from the fact that the channel has almost no free space for ion or water transport but generates a hydrogen bonded wire in the presence of protons to allow the proton hopping. Inspired by this, we used the interlayer spac...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Qi Li Hongfei Gao Yongye Zhao Bo Zhou Lei Yu Qingsong Huang Lei Jiang Jun Gao Source Type: research
Chemical synthesis of Acetobacter pasteurianus lipid A with a unique tetrasaccharide backbone and evaluation of its immunological functions
In this study, we focused on A. pasteurianus lipid A, which is a potential immunostimulatory component of kurozu. The active principle structure of A. pasteurianus lipid A has not yet been identified. Herein, we first systematically synthesized three types of A. pasteurianus lipid As containing a common and unique tetrasaccharide backbone. We developed an efficient method for constructing the 2-trehalosamine skeleton utilizing borinic acid-catalyzed glycosylation to afford 1,1'-α,α-glycoside in high yield and stereoselectivity. A common tetrasaccharide intermediate with an orthogonal protecting group pattern was construc...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Haruki Yamaura Atsushi Shimoyama Koji Hosomi Kazuya Kabayama Jun Kunisawa Koichi Fukase Source Type: research
One-Step Butadiene Purification in a Sulfonate-Functionalized Metal-Organic Framework through Synergistic Separation Mechanism
Angew Chem Int Ed Engl. 2024 Apr 5:e202403345. doi: 10.1002/anie.202403345. Online ahead of print.ABSTRACTPorous materials that could recognize specific molecules from complex mixtures are of great potential in improving the current energy-intensive multistep separation processes. However, due to the highly similar structures and properties of the mixtures, the design of desired porous materials remains challenging. Herein, a sulfonate-functionalized metal-organic framework ZU-609 with suitable pore size and pore chemistry is designed for 1,3-butadiene (C4H6) purification from complex C4 mixtures. The sulfonate anions deco...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Jiyu Cui ZhenSong Qiu Zhenglu Yang Anye Jin Xili Cui Lifeng Yang Huabin Xing Source Type: research
Temperature-Controlled Selective Formation of Silver Nanoclusters and Their Transformation to the Same Product
Angew Chem Int Ed Engl. 2024 Apr 5:e202403464. doi: 10.1002/anie.202403464. Online ahead of print.ABSTRACTHerein, two atomically precise silver nanoclusters, Ag54 and Ag33, directed by inner anion templates (CrO42- and/or Cl-), are initially isolated as a mixed phase from identical reactants across a wide temperature range (20-80 °C). Interestingly, fine-tuning the reaction temperature can realize pure phase synthesis of the two nanoclusters; that is, a metastable Ag54 is kinetically formed at a low temperature (20 °C), whereas such a system is steered towards a thermodynamically stable Ag33 at a relatively high temperat...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Zhi Wang Yuchen Wang Tian-Yang Xu Li Li Christine M Aikens Zhi-Yong Gao Mohammad Azam Chen-Ho Tung Di Sun Source Type: research
Tandem Catalysts Enabling Efficient C-N Coupling toward the Electrosynthesis of Urea
This study provides an effective avenue for the design and synthesis of tandem catalysts for electrocatalytic urea synthesis.PMID:38581164 | DOI:10.1002/anie.202402215 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Yuhang Gao Jingnan Wang Menglong Sun Yuan Jing Lili Chen Zhiqin Liang Yijun Yang Chuang Zhang Jiannian Yao Xi Wang Source Type: research
Single-Atom Titanium on Mesoporous Nitrogen, Oxygen-Doped Carbon for Efficient Photo-thermal Catalytic CO2 Cycloaddition by a Radical Mechanism
Angew Chem Int Ed Engl. 2024 Apr 6:e202404911. doi: 10.1002/anie.202404911. Online ahead of print.ABSTRACTDeveloping efficient and earth-abundant catalysts for CO2 fixation to high value-added chemicals is meaningful but challenging. Styrene carbonate has great market value, but the cycloaddition of CO2 to styrene oxide is difficult due to the high steric hindrance and weak electron-withdrawing ability of the phenyl group. To utilize clean energy (such as optical energy) directly and effectively for CO2 value-added process, we introduce earth-abundant Ti single-atom into the mesoporous nitrogen, oxygen-doped carbon nanoshe...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Yifan Wang Huimin Liu Qiujin Shi Zerui Miao Haohong Duan Yiou Wang Hongpan Rong Jiatao Zhang Source Type: research
Elucidation of Palmarumycin Spirobisnaphthalene Biosynthesis Reveals a Set of Previously Unrecognized Oxidases and Reductases
In this study, we elucidated the biosynthesis of palmarumycins, using gene disruption, heterologous expression, and substrate feeding experiments. The biosynthetic gene cluster for palmarumycins was identified to be distant from the polyketide synthase gene cluster, and included two cytochrome P450s (PalA and PalB), and one short chain dehydrogenase/reductase (PalC) encoding genes as key structural genes. PalA is an unusual, multifunctional P450 that catalyzes the oxidative dimerization of 1,8-dihydroxynaphthalene to generate the spiroketal linkage and 2,3-epoxy group. Chemical synthesis of key intermediate and in vitro bi...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Siji Zhao Zhen Shen Ziqi Zhai Ruya Yin Dan Xu Mingan Wang Qi Wang You-Liang Peng Ligang Zhou Daowan Lai Source Type: research
Covalent Organic Framework Interlayer Spacings as Perfectly Selective Artificial Proton Channels
Angew Chem Int Ed Engl. 2024 Apr 6:e202402094. doi: 10.1002/anie.202402094. Online ahead of print.ABSTRACTBiological proton channels have perfect selectivity in aqueous environment against almost all ions and molecules, a property that differs itself from other biological channels and a feature that remains challenging to realize for bulk artificial materials. The biological perfect selectivity originates from the fact that the channel has almost no free space for ion or water transport but generates a hydrogen bonded wire in the presence of protons to allow the proton hopping. Inspired by this, we used the interlayer spac...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Qi Li Hongfei Gao Yongye Zhao Bo Zhou Lei Yu Qingsong Huang Lei Jiang Jun Gao Source Type: research
Chemical synthesis of Acetobacter pasteurianus lipid A with a unique tetrasaccharide backbone and evaluation of its immunological functions
In this study, we focused on A. pasteurianus lipid A, which is a potential immunostimulatory component of kurozu. The active principle structure of A. pasteurianus lipid A has not yet been identified. Herein, we first systematically synthesized three types of A. pasteurianus lipid As containing a common and unique tetrasaccharide backbone. We developed an efficient method for constructing the 2-trehalosamine skeleton utilizing borinic acid-catalyzed glycosylation to afford 1,1'-α,α-glycoside in high yield and stereoselectivity. A common tetrasaccharide intermediate with an orthogonal protecting group pattern was construc...
Source: Angewandte Chemie - April 6, 2024 Category: Chemistry Authors: Haruki Yamaura Atsushi Shimoyama Koji Hosomi Kazuya Kabayama Jun Kunisawa Koichi Fukase Source Type: research
Activable Nano-Immunomodulator Assembled from π-Extended Naphthalenediimide for Precision Photothermal Immunotherapy
Angew Chem Int Ed Engl. 2024 Apr 4:e202401250. doi: 10.1002/anie.202401250. Online ahead of print.ABSTRACTA nano-immunomodulator (R-NPT NP) comprising a tumor microenvironment (TME) activable resiquimod (R848) and a π-extended NIR-absorbing naphthophenanthrolinetetraone (NPT) has been engineered for spatiotemporal controlled photothermal immunotherapy. R-NPT NP demonstrated excellent photostability, while R848 promoted synergistic immunity as a toll-like receptor 7/8 (TLR7/8) agonist. Upon accumulation at the tumor site, R-NPT NP released R848 in response to redox metabolite glutathione (GSH), triggering dendritic cell (D...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Wenbin Zhong Wei Yuan Yun Chen Zhaoyu Ma Mengmeng Ma Brynne Shu Ni Tan Jie Yang Yanli Zhao Source Type: research
Neighbouring Synergy in High-density Single Ir Atoms on CoGaOOH for Efficient Alkaline Electrocatalytic Oxygen Evolution
Angew Chem Int Ed Engl. 2024 Apr 4:e202404418. doi: 10.1002/anie.202404418. Online ahead of print.ABSTRACTThe catalytic performance of single-atom catalysts was strictly limited by isolated single-atom sites. Fabricating high-density single atoms to realize the synergetic interaction in neighbouring single atoms could optimize the adsorption behaviors of reaction intermediates, which exhibited great potential to break performance limitations and deepen mechanistic understanding of electrocatalysis. However, the catalytic behavior governed by neighbouring single atoms is particularly elusive and has yet to be understood. He...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Peiyu Ma Heng Cao Qi Hao Ruyang Wang Wanting Liu Ming Zuo Chuanyi Jia Zhirong Zhang Jun Bao Source Type: research
Rational Design of Local Reaction Environment for Electrocatalytic Conversion of CO2 into Multicarbon Products
Angew Chem Int Ed Engl. 2024 Apr 4:e202401185. doi: 10.1002/anie.202401185. Online ahead of print.ABSTRACTThe electrocatalytic conversion of CO2 into multi-carbon (C2+) products provides an attractive route for storing intermittent renewable electricity as fuels and feedstocks with high energy densities. Although substantial progress has been made in selective electrosynthesis of C2+ products via engineering the catalyst, rational design of the local reaction environment in the vicinity of catalyst surface also acts as an effective approach for further enhancing the performance. Here, we discuss recent advances and pertine...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Ming Ma Brian Seger Source Type: research
Photo-responsive Hydrogen-Bonded Molecular Networks Capable of Retaining Crystalline Periodicity after Isomerization
This study describes a photo-responsive single crystal based on hydrogen-bonded (H-bonded) network of dihydrodimethylbenzo[e]pyrene derivative 4BDHP. A crystal composed of H-bonded undulate layers, 4BDHP-2, underwent photoisomerization in the crystalline state due to loose stacking of the layers, resulting loss of crystallinity. Enantio-pure crystal (S,S)-4BDHP-2, on the other hand, allowed to reveal the structure of the photoisomerized crystal, in which the closed form (4BDHP) and open form (4CPD) were arranged alternately with keeping crystalline periodicity, although side reactions were also implied. The present proof-o...
Source: Angewandte Chemie - April 5, 2024 Category: Chemistry Authors: Koki Kasuya Ryusei Oketani Souta Matsuda Hiroyasu Sato Fumitaka Ishiwari Akinori Saeki Ichiro Hisaki Source Type: research
