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941.
Yifan Feng Ruixuan Shi Mingfang Yang Yunlong Zheng Prof. Zhenjie Zhang Prof. Yao Chen 《Angewandte Chemie (International ed. in English)》2023,62(20):e202302436
Enzyme immobilization has been demonstrated to be a favorable protocol for promoting the industrialization of bioactive molecules, but still with formidable challenge. Addressing this challenge, we create a dynamic defect generation strategy for enzyme immobilization by using the dissociation equilibrium of metal-organic frameworks (MOFs) mediated by enzymes. Enzymes can act as “macro ligands” to generate competitive coordination against original ligands, along with the release of metal clusters of MOFs to generate defects, hence promoting the gradual transport of enzymes from the surface to inside. Various enzymes can be efficiently immobilized in MOFs to afford composites with good enzymatic activities, protective performances and exceptional reusabilities. Moreover, multienzyme bioreactors capable of efficient cascade reactions can also be generated. This study provides new opportunities to construct highly efficient biocatalysts incorporating different types of enzymes. 相似文献
942.
Luca C. Greiner Dr. Norihito Arichi Prof. Dr. Shinsuke Inuki Prof. Dr. Hiroaki Ohno 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(3):e202213653
Phenyl azides substituted by an (alkylphenyl)ethynyl group facilitate benzylic sp3(C−H) functionalization in the presence of a JohnPhosAu catalyst, resulting in indole-fused tetra- and pentacycles via divergent N- or C-cyclization. The chemoselectivity is influenced depending on the counter-anion, the electron density of the α-imino gold(I) carbene, and the alkyl groups stabilizing the benzylic carbocation originating from a 1,5-hydride shift. An isotopic labeling experiment demonstrates the involvement of an indolylgold(I) species resulting from a tautomerization that is much faster than the deauration. The formation of a benzylic sp3(C−H) functionalization leading to an indole-fused seven-membered ring is also demonstrated. 相似文献
943.
Dr. Leiming Guo Dr. Konstantinos Ntetsikas Dr. Georgios Zapsas Dr. Roshni Thankamony Prof. Zhiping Lai Prof. Nikos Hadjichristidis 《Angewandte Chemie (International ed. in English)》2023,62(4):e202212400
The great significance of boosting the design of percolating nanopore structures in block copolymers (BCPs) for various cases has been widely demonstrated in the past several decades. However, it still remains challenging to prepare the desired porous structures in a rapid, facile, and universal manner. Here we have developed an unconventional and benchtop strategy to rapidly generate the nanoporous polystyrene-based BCPs with arbitrary structural characteristics regardless of the BCP bulk morphology. This universal pore-forming strategy enables the sustainable CO2-based BCPs to form advanced membranes after 1 s soaking for efficiently rejecting 94.2 % brilliant blue R (826 g mol−1). Meanwhile, the water permeance retains around 1020 L (m2 h bar)−1, which is 1–3 orders of magnitude higher than that of other membranes. This strategy may offer an excellent opportunity to introduce percolating pore structures in those newly developed BCPs with which the previously reported pore-forming methods may not deal. 相似文献
944.
Siew Kheng Boong Carice Chong Jinn-Kye Lee Zhi Zhong Ang Dr. Haitao Li Prof. Hiang Kwee Lee 《Angewandte Chemie (International ed. in English)》2023,62(7):e202216562
Plasmonic catalysis promises green ammonia synthesis but is limited by the need for co-catalysts and poor performances due to weak electromagnetic field enhancement. Here, we use two-dimensional plasmonic superlattices with dense electromagnetic hotspots to boost ambient nitrogen-to-ammonia photoconversion without needing co-catalyst. By organizing Ag octahedra into a square superlattice to concentrate light, the ammonia formation is enhanced by ≈15-fold and 4-fold over hexagonal superlattice and disorganized array, respectively. Our unique catalyst achieves superior ammonia formation rate and apparent quantum yield up to ≈15-fold and ≈103-fold, respectively, better than traditional designs. Mechanistic investigations reveal the abundance of intense plasmonic hotspots is crucial to promote hot electron generation and transfer for nitrogen reduction. Our work offers valuable insights to design electromagnetically hot plasmonic catalysts for diverse chemical and energy applications. 相似文献
945.
Dr. Shangfa Pan Prof. Peng Liu Qi Li Bin Zhu Prof. Xueli Liu Junchao Lao Prof. Jun Gao Prof. Lei Jiang 《Angewandte Chemie (International ed. in English)》2023,62(19):e202218129
Nanofluidic membranes have shown great promise in harvesting osmotic energy but its scalablity remains challenging since most studies only tested with a membrane area of ≈10−2 mm2 or smaller. We demonstrate that metal-organic-framework membranes with subnanometer pores can be used for scalable osmotic power generation from hypersaline water sources. Our membrane can be scaled up to a few mm2, and the power density can be stabilized at 1.7 W m−2. We reveal that the key is to improve the out-of-membrane conductance while keeping the membrane's charge selectivity, contradicting the previous conception that the ionic conductivity of the membrane plays the dominating role. We highlight that subnanometer pores are essential to ensure the charge selectivity in hypersaline water sources. Our results suggest the importance to engineer the interplay between the in-membrane and out-of-membrane ion transport properties for scalable osmotic power generation. 相似文献
946.
Dr. Rui-An Li Qian-Qian Liu Xin Liu Dr. Youquan Liu Prof. Xingxing Jiang Prof. Zheshuai Lin Dr. Fei Jia Dr. Lin Xiong Prof. Ling Chen Prof. Li-Ming Wu 《Angewandte Chemie (International ed. in English)》2023,62(7):e202218048
The strong mutual coupling of and even the opposite change in the key parameters, such as the band gap (Eg) and second-order harmonic generation (SHG), leads to the extreme scarcity in high-performance IR nonlinear optical (NLO) chalcogenides. Herein, we report 8 new sulfides, Na2Ba[(AgxNa1−x)2Sn2S7] ( 1 , x=0; 1 series , x=0.1–0.6; Na2Ba[(Li0.58Na0.42)2Sn2S7], 1-0.6Li ); Na2Sr[Cu2Sn2S7] ( 2 ); and Na2Ba[Cu2Sn2S7] ( 3 ). We use the structural tolerance factor ( ) to connect the chemical composition, crystal structure, and NLO properties. Guided by these correlations, a better balance between Eg and SHG is realized in 1 , which exhibits a large Eg of 3.42 eV and excellent NLO properties (SHG: 1.5×AGS; laser-induced damage threshold: 12×AGS), representing the best performance among the known Hg- or As-free sulfides to date. 相似文献