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61.
Dr. Yinxiang Zeng Zhihao Pei Dr. Yan Guo Dr. Deyan Luan Prof. Xiaojun Gu Prof. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2023,62(45):e202312145
Constructing multifunctional interphases to suppress the rampant Zn dendrite growth and detrimental side reactions is crucial for Zn anodes. Herein, a phytic acid (PA)-ZnAl coordination compound is demonstrated as a versatile interphase layer to stabilize Zn anodes. The zincophilic PA-ZnAl layer can manipulate Zn2+ flux and promote rapid desolvation kinetics, ensuring the uniform Zn deposition with dendrite-free morphology. Moreover, the robust PA-ZnAl protective layer can effectively inhibit the hydrogen evolution reaction and formation of byproducts, further contributing to the reversible Zn plating/stripping with high Coulombic efficiency. As a result, the Zn@PA-ZnAl electrode shows a lower Zn nucleation overpotential and higher Zn2+ transference number compared with bare Zn. The Zn@PA-ZnAl symmetric cell exhibits a prolonged lifespan of 650 h tested at 5 mA cm−2 and 5 mAh cm−2. Furthermore, the assembled Zn battery full cell based on this Zn@PA-ZnAl anode also delivers decent cycling stability even under harsh conditions. 相似文献
62.
Jingcheng Wu Leitao Xu Zhijie Kong Kaizhi Gu Yuxuan Lu Xianwen Wu Prof. Yuqin Zou Prof. Shuangyin Wang 《Angewandte Chemie (International ed. in English)》2023,62(45):e202311196
Alanine is widely employed for synthesizing polymers, pharmaceuticals, and agrochemicals. Electrocatalytic coupling of biomass molecules and waste nitrate is attractive for the nitrate removal and alanine production under ambient conditions. However, the reaction efficiency is relatively low due to the activation of the stable substrates, and the coupling of two reactive intermediates remains challenging. Herein, we realize the integrated tandem electrochemical-chemical-electochemical synthesis of alanine from the biomass-derived pyruvic acid (PA) and waste nitrate (NO3−) catalyzed by PdCu nano-bead-wires (PdCu NBWs). The overall reaction pathway is demonstrated as a multiple-step catalytic cascade process via coupling the reactive intermediates NH2OH and PA on the catalyst surface. Interestingly, in this integrated tandem electrochemical-chemical-electrochemical catalytic cascade process, Cu facilitates the electrochemical reduction of nitrate to NH2OH intermediates, which chemically couple with PA to form the pyruvic oxime, and Pd promotes the electrochemical reduction of pyruvic oxime to the desirable alanine. This work provides a green strategy to convert waste NO3− to wealth and enriches the substrate scope of renewable biomass feedstocks to produce high-value amino acids. 相似文献
63.
Ziwei Xu Hongwei Dong Dr. Wanmiao Gu Dr. Zhen He Fengming Jin Dr. Chengming Wang Dr. Qing You Prof. Dr. Jin Li Prof. Dr. Haiteng Deng Dr. Lingwen Liao Dr. Dong Chen Prof. Dr. Jun Yang Prof. Dr. Zhikun Wu 《Angewandte Chemie (International ed. in English)》2023,62(39):e202308441
Lattice tuning at the ≈1 nm scale is fascinating and challenging; for instance, lattice compression at such a minuscule scale has not been observed. The lattice compression might also bring about some unusual properties, which waits to be verified. Through ligand induction, we herein achieve the lattice compression in a ≈1 nm gold nanocluster for the first time, as detected by the single-crystal X-ray crystallography. In a freshly synthesized Au52(CHT)28 (CHT=S-c−C6H11) nanocluster, the lattice distance of the (110) facet is found to be compressed from 4.51 to 3.58 Å at the near end. However, the lattice distances of the (111) and (100) facets show no change in different positions. The lattice-compressed nanocluster exhibits superior electrocatalytic activity for the CO2 reduction reaction (CO2RR) compared to that exhibited by the same-sized Au52(TBBT)32 (TBBT=4-tert-butyl-benzenethiolate) nanocluster and larger Au nanocrystals without lattice variation, indicating that lattice tuning is an efficient method for tailoring the properties of metal nanoclusters. Further theoretical calculations explain the high CO2RR performance of the lattice-compressed Au52(CHT)28 and provide a correlation between its structure and catalytic activity. 相似文献
64.
Dr. Yunxiang Li Dr. Yan Guo Dr. Deyan Luan Prof. Xiaojun Gu Prof. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2023,62(44):e202310847
Developing highly efficient catalytic sites for O2 reduction to H2O2, while ensuring the fast injection of energetic electrons into these sites, is crucial for artificial H2O2 photosynthesis but remains challenging. Herein, we report a strongly coupled hybrid photocatalyst comprising polymeric carbon nitride (CN) and a two-dimensional conductive Zn-containing metal–organic framework (Zn-MOF) (denoted as CN/Zn-MOF(lc)/400; lc, low crystallinity; 400, annealing temperature in °C), in which the catalytic capability of Zn-MOF(lc) for H2O2 production is unlocked by the annealing-induced effects. As revealed by experimental and theoretical calculation results, the Zn sites coordinated to four O (Zn-O4) in Zn-MOF(lc) are thermally activated to a relatively electron-rich state due to the annealing-induced local structure shrinkage, which favors the formation of a key *OOH intermediate of 2e− O2 reduction on these sites. Moreover, the annealing treatment facilitates the photoelectron migration from the CN photocatalyst to the Zn-MOF(lc) catalytic unit. As a result, the optimized catalyst exhibits dramatically enhanced H2O2 production activity and excellent stability under visible light irradiation. 相似文献
65.
Si-Yong Yin Qiansujia Zhou Dr. Chen-Xu Liu Prof. Dr. Qing Gu Prof. Dr. Shu-Li You 《Angewandte Chemie (International ed. in English)》2023,62(37):e202305067
Enantioselective synthesis of N−N biaryl atropisomers is an emerging area but remains underexplored. The development of efficient synthesis of N−N biaryl atropisomers is in great demand. Herein, the construction of N−N biaryl atropisomers through iridium-catalyzed asymmetric C−H alkylation is reported for the first time. In the presence of readily available Ir precursor and Xyl-BINAP, a variety of axially chiral molecules based on indole-pyrrole skeleton were obtained in good yields (up to 98 %) with excellent enantioselectivity (up to 99 % ee). In addition, N−N bispyrrole atropisomers could also be synthesized in excellent yields and enantioselectivity. This method features perfect atom economy, wide substrate scope, and multifunctionalized products allowing diverse transformations. 相似文献
66.
Dr. Wen-Da Zhang Lang Zhou Ya-Xiang Shi Dr. Yong Liu Hanwen Xu Prof. Dr. Xiaodong Yan Yan Zhao Prof. Dr. Yuqin Jiang Prof. Dr. Jiangwei Zhang Prof. Dr. Zhi-Guo Gu 《Angewandte Chemie (International ed. in English)》2023,62(27):e202304412
Dual-atom catalysts (DAC) are deemed as promising electrocatalysts due to the abundant active sites and adjustable electronic structure, but the fabrication of well-defined DAC is still full of challenges. Herein, bonded Fe dual-atom catalysts (Fe2DAC) with Fe2N6C8O2 configuration were developed through one-step carbonization of a preorganized covalent organic framework with bimetallic Fe chelation sites (Fe2COF). The transition from Fe2COF to Fe2DAC involved the dissociation of the nanoparticles and the capture of atoms by carbon defects. Benefitting from the optimized d-band center and enhanced adsorption of OOH* intermediates, Fe2DAC exhibited outstanding oxygen reduction activity with a half-wave potential of 0.898 V vs. RHE. This work will guide more fabrication of dual-atom and even cluster catalysts from preorganized COF in the future. 相似文献
67.
Weiqing Xu Yu Wu Yuling Xu Dr. Xiaoli Cai Prof. Wenling Gu Prof. Chengzhou Zhu 《Angewandte Chemie (International ed. in English)》2023,62(47):e202308827
Enzymatic catalysis with high efficiency allows them a great prospect in metabolite monitoring in living cells. However, complex tumor microenvironments, such as acidity, H2O2, and hypoxia, are bound to disturb catalytic reactions for misleading results. Here, we report a spatially compartmentalized artificial organelle to correct intratumoral glucose analysis, where the zeolitic imidazolate framework-8 immobilized glucose oxidase-horseradish peroxidase cascade core and catalase-directed shell act as signal transduction and guarding rooms respectively. The acid-digested core and stable shell provide appropriate spaces to boost biocatalytic efficiency with good tolerability. Notably, the endogenous H2O2 is in situ decomposed to O2 by catalase, which not only overcomes the interference in signal output but also alleviates the hypoxic states to maximize glucose oxidation. The marked protective effect and biocompatibility render artificial organelles to correct the signal transduction for dynamic monitoring glucose in vitro and in vivo, achieving our goal of accurate intratumoral metabolite analysis. 相似文献
68.
Prof. Xiaona Li Yang Xu Prof. Changtai Zhao Duojie Wu Dr. Limin Wang Matthew Zheng Xu Han Dr. Simeng Zhang Junyi Yue Prof. Biwei Xiao Dr. Wei Xiao Dr. Ligen Wang Prof. Tao Mei Prof. Meng Gu Prof. Jianwen Liang Prof. Xueliang Sun 《Angewandte Chemie (International ed. in English)》2023,62(48):e202306433
As exciting candidates for next-generation energy storage, all-solid-state lithium batteries (ASSLBs) are highly dependent on advanced solid-state electrolytes (SSEs). Here, using cost-effective LaCl3 and CeCl3 lattice (UCl3-type structure) as the host and further combined with a multiple-cation mixed strategy, we report a series of UCl3-type SSEs with high room-temperature ionic conductivities over 10−3 S cm−1 and good compatibility with high-voltage oxide cathodes. The intrinsic large-size hexagonal one-dimensional channels and highly disordered amorphous phase induced by multi-metal cation species are believed to trigger fast multiple ionic conductions of Li+, Na+, K+, Cu+, and Ag+. The UCl3-type SSEs enable a stable prototype ASSLB capable of over 3000 cycles and high reversibility at −30 °C. Further exploration of the brand-new multiple-cation mixed chlorides is likely to lead to the development of advanced halide SSEs suitable for ASSLBs with high energy density. 相似文献
69.
Hydrogen spillover, involving the surface migration of dissociated hydrogen atoms from active metal sites to the relatively inert catalyst support, plays a crucial role in hydrogen-involved catalytic processes. However, a comprehensive understanding of how H atoms are driven to spill over from active sites onto the catalyst support is still lacking. Here, we examine the atomic-scale perspective of the H spillover process on a Pt/Cu(111) single atom alloy surface using machine-learning accelerated molecular dynamics calculations based on density functional theory. Our results show that when an impinging H2 dissociates at an active Pt site, the Pt atom undergoes deactivation due to the dissociated hydrogen atoms that attach to it. Interestingly, collisions between H2 and sticking H atoms facilitate H spillover onto the host Cu, leading to the reactivation of the Pt atom and the realization of a continuous H spillover process. This work underscores the importance of the interaction between gas molecules and adsorbates as a driving force in elucidating chemical processes under a gaseous atmosphere, which has so far been underappreciated in thermodynamic studies. 相似文献
70.
Dr. Ningxia Gu Zeyuan Sun Dr. Lixin Song Prof. Dr. Pingfan Du Prof. Dr. Jie Xiong 《Chemphyschem》2023,24(14):e202200919
The perovskite solar cells (PSCs) with high efficiency and stability are in great demand for commercial applications. Although the remarkable photovoltaic feature of perovskite layer plays a great role in improving the PCE of PSCs, the inevitable defects and poor stability of perovskite, etc. are the bottleneck and restrict the commercialization of PSCs. Herein, a review provides a strategy of applying aggregation-induced emission (AIE) molecules, containing passivation functional groups and distinct AIE character, which serves as the alternative materials for fabricating high-efficiency and high-stability PSCs. The methods of introducing AIE molecules to PSCs are also summarized, including additive engineering, interfacial engineering, hole transport materials and so on. In addition, the functions of AIE molecule are discussed, such as defects passivation, morphology modulation, well-matched energy level, enhanced stability, hole transport ability, carrier recombination suppression. Finally, the detailed functions of AIE molecules are offered and further research trend for high performance PSCs based on AIE materials is proposed. 相似文献