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991.
Taotao Wang Li Zhang Jinbao Wu Prof. Muqing Chen Prof. Shangfeng Yang Prof. Yalin Lu Prof. Pingwu Du 《Angewandte Chemie (International ed. in English)》2023,62(40):e202311352
A few-layer fullerene network possesses several advantageous characteristics, including a large surface area, abundant active sites, high charge mobility, and an appropriate band gap and band edge for solar water splitting. Herein, we report for the first time that the few-layer fullerene network shows interesting photocatalytic performance in pure water splitting into H2 and H2O2 in the absence of any sacrificial reagents. Under optimal conditions, the H2 and H2O2 evolution rates can reach 91 and 116 μmol g−1 h−1, respectively, with good stability. This work demonstrates the novel application of the few-layer fullerene network in the field of energy conversion. 相似文献
992.
Qiao Zhang Hsin Jung Tsai Fuhua Li Zhiming Wei Qinye He Dr. Jie Ding Yuhang Liu Zih-Yi Lin Xiaoju Yang Dr. Zhaoyang Chen Prof. Fangxin Hu Prof. Xuan Yang Prof. Qing Tang Prof. Hong Bin Yang Prof. Sung-Fu Hung Prof. Yueming Zhai 《Angewandte Chemie (International ed. in English)》2023,62(44):e202311550
Single-atom catalysts exhibit superior CO2-to-CO catalytic activity, but poor kinetics of proton-coupled electron transfer (PCET) steps still limit the overall performance toward the industrial scale. Here, we constructed a Fe−P atom paired catalyst onto nitrogen doped graphitic layer (Fe1/PNG) to accelerate PCET step. Fe1/PNG delivers an industrial CO current of 1 A with FECO over 90 % at 2.5 V in a membrane-electrode assembly, overperforming the CO current of Fe1/NG by more than 300 %. We also decrypted the synergistic effects of the P atom in the Fe−P atom pair using operando techniques and density functional theory, revealing that the P atom provides additional adsorption sites for accelerating water dissociation, boosting the hydrogenation of CO2, and enhancing the activity of CO2 reduction. This atom-pair catalytic strategy can modulate multiple reactants and intermediates to break through the inherent limitations of single-atom catalysts. 相似文献
993.
Hui Liang Manlin Lu Zafar Mahmood Zheng Li Zeduan Chen Guowei Chen Prof. Ming-De Li Prof. Yanping Huo Prof. Shaomin Ji 《Angewandte Chemie (International ed. in English)》2023,62(44):e202312600
The design of efficient heavy atom-free triplet photosensitizers (PSs) based on through bond charge transfer (TBCT) features is a formidable challenge due to the criteria of orthogonal donor-acceptor geometry. Herein, we propose using parallel (face-to-face) conformation carbazole-bodipy donor-acceptor dyads (BCZ-1 and BCZ-2) featuring through space intramolecular charge transfer (TSCT) process as efficient triplet PS. Efficient intersystem crossing (ΦΔ=61 %) and long-lived triplet excited state (τT=186 μs) were observed in the TSCT dyad BCZ-1 compared to BCZ-3 (ΦΔ=0.4 %), the dyad involving TBCT, demonstrating the superiority of the TSCT approach over conventional donor-acceptor system. Moreover, the transient absorption study revealed that TSCT dyads have a faster charge separation and slower intersystem crossing process induced by charge recombination compared to TBCT dyad. A long-lived charge-separated state (CSS) was observed in the BCZ-1 (τCSS=24 ns). For the first time, the TSCT dyad was explored for the triplet-triplet annihilation upconversion, and a high upconversion quantum yield of 11 % was observed. Our results demonstrate a new avenue for designing efficient PSs and open up exciting opportunities for future research in this field. 相似文献
994.
Dr. Ying-Jie Sun Wen-Da Chen Dr. Ji Liu Jun-Jin Li Yu Zhang Wei-Qi Cai Prof. Li Liu Xin-Jing Tang Jian Hou Prof. Ming Wang Prof. Liang Cheng 《Angewandte Chemie (International ed. in English)》2023,62(5):e202212413
The CRISPR/Cas system is one of the most powerful tools for gene editing. However, approaches for precise control of genome editing and regulatory events are still desirable. Here, we report the spatiotemporal and efficient control of CRISPR/Cas9- and Cas12a-mediated editing with conformationally restricted guide RNAs (gRNAs). This approach relied on only two or three pre-installed photo-labile substituents followed by an intramolecular cyclization, representing a robust synthetic method in comparison to the heavily modified linear gRNAs that often require extensive screening and time-consuming optimization. This tactic could direct the precise cleavage of the genes encoding green fluorescent protein (GFP) and the vascular endothelial growth factor A (VEGFA) protein within a predefined cutting region without notable editing leakage in live cells. We also achieved light-mediated myostatin (MSTN) gene editing in embryos, wherein a new bow-knot-type gRNA was constructed with excellent OFF/ON switch efficiency. Overall, our work provides a significant new strategy in CRISPR/Cas editing with modified circular gRNAs to precisely manipulate where and when genes are edited. 相似文献
995.
Yutong Pi Linxia Cui Prof. Wenhao Luo Dr. Haitao Li Dr. Yanfu Ma Dr. Na Ta Xinyao Wang Prof. Rui Gao Prof. Dan Wang Prof. Qihua Yang Prof. Jian Liu 《Angewandte Chemie (International ed. in English)》2023,62(43):e202307096
Mimicking the structures and functions of cells to create artificial organelles has spurred the development of efficient strategies for production of hollow nanoreactors with biomimetic catalytic functions. However, such structure are challenging to fabricate and are thus rarely reported. We report the design of hollow nanoreactors with hollow multishelled structure (HoMS) and spatially loaded metal nanoparticles. Starting from a molecular-level design strategy, well-defined hollow multishelled structure phenolic resins (HoMS-PR) and carbon (HoMS-C) submicron particles were accurately constructed. HoMS-C serves as an excellent, versatile platform, owing to its tunable properties with tailored functional sites for achieving precise spatial location of metal nanoparticles, internally encapsulated (Pd@HoMS-C) or externally supported (Pd/HoMS-C). Impressively, the combination of the delicate nanoarchitecture and spatially loaded metal nanoparticles endow the pair of nanoreactors with size–shape-selective molecular recognition properties in catalytic semihydrogenation, including high activity and selectivity of Pd@HoMS-C for small aliphatic substrates and Pd/HoMS-C for large aromatic substrates. Theoretical calculations provide insight into the pair of nanoreactors with distinct behaviors due to the differences in energy barrier of substrate adsorption. This work provides guidance on the rational design and accurate construction of hollow nanoreactors with precisely located active sites and a finely modulated microenvironment by mimicking the functions of cells. 相似文献
996.
Yaxin Zeng Prof. Dr. Ying Xia 《Angewandte Chemie (International ed. in English)》2023,62(32):e202307129
Direct synthesis of gem-difluorinated carbocyclic molecules represents a longstanding challenge in organic chemistry. Herein, a Rh-catalyzed [3+2] cycloaddition reaction between readily available gem-difluorinated cyclopropanes (gem-DFCPs) and internal olefins has been developed, enabling the efficient synthesis of gem-difluorinated cyclopentanes with good functional group compatibility, excellent regioselectivity and good diastereoselectivity. The resulting gem-difluorinated products can undergo downstream transformations to access various mono-fluorinated cyclopentenes and cyclopentanes. This reaction demonstrates the use of gem-DFCPs as a type of “CF2” C3 synthon for cycloaddition under transition metal catalysis, which provides potential strategy for synthesizing other gem-difluorinated carbocyclic molecules. 相似文献
997.
Xin Feng Dr. Kejun Bu Teng Liu Songhao Guo Zongdong Sun Tonghuan Fu Yongshan Xu Dr. Kailang Liu Dr. Sijie Yang Dr. Yinghe Zhao Prof. Huiqiao Li Prof. Xujie Lü Prof. Tianyou Zhai 《Angewandte Chemie (International ed. in English)》2023,62(9):e202217238
The unique intermolecular van der Waals force in emerging two-dimensional inorganic molecular crystals (2DIMCs) endows them with highly tunable structures and properties upon applying external stimuli. Using high pressure to modulate the intermolecular bonding, here we reveal the highly tunable charge transport behavior in 2DIMCs for the first time, from an insulator to a semiconductor. As pressure increases, 2D α-Sb2O3 molecular crystal undergoes three isostructural transitions, and the intermolecular bonding enhances gradually, which results in a considerably decreased band gap by 25 % and a greatly enhanced charge transport. Impressively, the in situ resistivity measurement of the α-Sb2O3 flake shows a sharp drop by 5 orders of magnitude in 0–3.2 GPa. This work sheds new light on the manipulation of charge transport in 2DIMCs and is of great significance for promoting the fundamental understanding and potential applications of 2DIMCs in advanced modern technologies. 相似文献
998.
Hong-Jun Liu Cheng-Ye Yang Mei-Chen Han Chun-Yu Yu Prof. Xiaofeng Li Prof. Zhong-Zhen Yu Prof. Jin Qu 《Angewandte Chemie (International ed. in English)》2023,62(11):e202217458
Constructing efficient artificial solid electrolyte interface (SEI) film is extremely vital for the practical application of lithium metal batteries. Herein, a dense artificial SEI film, in which lithiophilic Zn/LixZny are uniformly but nonconsecutively dispersed in the consecutive Li+-conductors of LixSiOy, Li2O and LiOH, is constructed via the in situ reaction of layered zinc silicate nanosheets and Li. The consecutive Li+-conductors can promote the desolvation process of solvated-Li+ and regulate the transfer of lithium ions. The nonconsecutive lithiophilic metals are polarized by the internal electric field to boost the transfer of lithium ions, and lower the nucleation barrier. Therefore, a low polarization of ≈50 mV for 750 h at 2.0 mA cm−2 in symmetric cells, and a high capacity retention of 99.2 % in full cells with a high lithium iron phosphate areal loading of ≈13 mg cm−2 are achieved. This work offers new sights to develop advanced alkali metal anodes for efficient energy storage. 相似文献
999.
Feifan Li Xinyang Mu Xueqing Tang Ge Song Hongzhao Sun Xiuling Zha Peiyan Sun Jianhui Fang Dongmei Hu Shan Cong Zhigang Zhao 《Angewandte Chemie (International ed. in English)》2023,62(12):e202218055
Non-metallic materials have emerged as a new family of active substrates for surface-enhanced Raman scattering (SERS), with unique advantages over their metal counterparts. However, owing to their inefficient interaction with the incident wavelength, the Raman enhancement achieved with non-metallic materials is considerably lower with respect to the metallic ones. Herein, we propose colourful semiconductor-based SERS substrates for the first time by utilizing a Fabry-Pérot cavity, which realize a large freedom in manipulating light. Owing to the delicate adjustment of the absorption in terms of both frequency and intensity, resonant absorption can be achieved with a variety of non-metal SERS substrates, with the sensitivity further enhanced by ≈100 times. As a typical example, by introducing a Fabry-Pérot-type substrate fabricated with SiO2/Si, a rather low detection limit of 10−16 M for the SARS-CoV-2S protein is achieved on SnS2. This study provides a realistic strategy for increasing SERS sensitivity when semiconductors are employed as SERS substrates. 相似文献
1000.
Cong Liu Chunshao Mo Linfeng Zhong Xiaoqi Gong Yang Zhang Xiaotong Wang Fan Yang Jing Li Prof. Jiang Lu Prof. Dingshan Yu 《Angewandte Chemie (International ed. in English)》2023,62(43):e202312016
Here, we for the first time introduce ethoxylation chemistry to develop a new octupolar cyano-vinylene-linked 2D polymer framework (Cyano-OCF-EO) capable of acting as efficient mixed electron/ion conductors and metal-free sulfur evolution catalysts for dual-promoted Li and S electrochemistry. Our strategy creates a unique interconnected network of strongly-coupled donor 3-(acceptor-core) octupoles in Cyano-OCF-EO, affording enhanced intramolecular charge transfer, substantial active sites and crowded open channels. This enables Cyano-OCF-EO as a new versatile separator modifier, which endows the modified separator with superior catalytic activity for sulfur conversion and rapid Li ion conduction with the high Li+ transference number up to 0.94. Thus, the incorporation of Cyano-OCF-EO can concurrently regulate sulfur redox reactions and Li-ion flux in Li−S cells, attaining boosted bidirectional redox kinetics, inhibited polysulfide shuttle and dendrite-free Li anodes. The Cyano-OCF-EO-involved Li−S cell is endowed with excellent overall electrochemical performance especially large areal capacity of 7.5 mAh cm−2 at high sulfur loading of 8.7 mg cm−2. Mechanistic studies unveil the dominant multi-promoting effect of the triethoxylation on electron and ion conduction, polysulfide adsorption and catalytic conversion as well as previously-unexplored −CN/C−O dual-site synergistic effect for enhanced polysulfide adsorption and reduced energy barrier toward Li2S conversion. 相似文献