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81.
Dr. Jin Su Dr. Tohru Tsuruoka Dr. Takuji Tsujita Dr. Yuu Inatomi Dr. Kazuya Terabe 《Angewandte Chemie (International ed. in English)》2023,62(9):e202217203
Solid-state batteries (SSBs) that use solid electrolytes instead of flammable liquid electrolytes have the potential to generate higher specific capacity and offer better safety. Magnesium (Mg) based SSBs with Mg metal anodes are considered to be one of the most promising energy storage candidates, because it gives high theoretical volumetric capacities of 3830 mAh cm−3. Here, we demonstrate an atomic layer deposition (ALD) process with a double nitrogen plasma process that successfully produces nitrogen-incorporated magnesium phosphorus oxynitride (MgPON) solid-state electrolyte (SSE) thin films at a low deposition temperature of 125 °C. The ALD MgPON SSEs exhibit an ionic conductivity of 0.36 and 1.2 μS cm−1 at 450 and 500 °C, respectively. The proposed ALD strategy shows the ability of conformal deposition nitrogen-doped SSEs on pattered substrates and is attractive for using nitride ion-conducing films as protective or wetting interlayers in solid-state Mg and Li batteries. 相似文献
82.
Dr. Xianzhong Yang Weiping Li Ziyan Chen Dr. Meng Tian Jun Peng Jinrong Luo Yiwen Su Yuhan Zou Gao Weng Prof. Yuanlong Shao Prof. Shixue Dou Prof. Jingyu Sun 《Angewandte Chemie (International ed. in English)》2023,62(10):e202218454
Despite conspicuous merits of Zn metal anodes, the commercialization is still handicapped by rampant dendrite formation and notorious side reaction. Manipulating the nucleation mode and deposition orientation of Zn is a key to rendering stabilized Zn anodes. Here, a dual electrolyte additive strategy is put forward via the direct cooperation of xylitol (XY) and graphene oxide (GO) species into typical zinc sulfate electrolyte. As verified by molecular dynamics simulations, the incorporated XY molecules could regulate the solvation structure of Zn2+, thus inhibiting hydrogen evolution and side reactions. The self-assembled GO layer is in favor of facilitating the desolvation process to accelerate reaction kinetics. Progressive nucleation and orientational deposition can be realized under the synergistic modulation, enabling a dense and uniform Zn deposition. Consequently, symmetric cell based on dual additives harvests a highly reversible cycling of 5600 h at 1.0 mA cm−2/1.0 mAh cm−2. 相似文献
83.
Dr. Yang Wei Dr. Yue Pan Dr. Enlong Zhou Dr. Ze Yuan Dr. Hao Song Dr. Yilin Wang Dr. Jie Zhou Jiahui Rui Mengjiao Xu Prof. Lixin Ning Dr. Zhanning Liu Dr. Hongyu Wang Prof. Xiaoji Xie Prof. Xiaobin Tang Prof. Haiquan Su Xianran Xing Prof. Ling Huang 《Angewandte Chemie (International ed. in English)》2023,62(27):e202303482
Although large amount of effort has been invested in combating thermal quenching that severely degrades the performance of luminescent materials particularly at high temperatures, not much affirmative progress has been realized. Herein, we demonstrate that the Frenkel defect formed via controlled annealing of Sc2(WO4)3:Ln (Ln=Yb, Er, Eu, Tb, Sm), can work as energy reservoir and back-transfer the stored excitation energy to Ln3+ upon heating. Therefore, except routine anti-thermal quenching, thermally enhanced 415-fold downshifting and 405-fold upconversion luminescence are even obtained in Sc2(WO4)3:Yb/Er, which has set a record of both the Yb3+-Er3+ energy transfer efficiency (>85 %) and the working temperature at 500 and 1073 K, respectively. Moreover, this design strategy is extendable to other hosts possessing Frenkel defect, and modulation of which directly determines whether enhanced or decreased luminescence can be obtained. This discovery has paved new avenues to reliable generation of high-temperature luminescence. 相似文献
84.
Yao Wu Cong Zhao Yanzhuang Su Prof. Dr. Sason Shaik Prof. Dr. Wenzhen Lai 《Angewandte Chemie (International ed. in English)》2023,62(7):e202212053
The copper-dependent formylglycine-generating enzyme (FGE) catalyzes the oxygen-dependent oxidation of specific peptidyl-cysteine residues to formylglycine. Our QM/MM calculations provide a very likely mechanism for this transformation. The reaction starts with dioxygen binding to the tris-thiolate CuI center to form a triplet CuII-superoxide complex. The rate-determining hydrogen atom abstraction involves a triplet-singlet crossing to form a CuII−OOH species that couples with the substrate radical, leading to a CuI-alkylperoxo intermediate. This is accompanied by proton transfer from the hydroperoxide to the S atom of the substrate via a nearby water molecule. The subsequent O−O bond cleavage is coupled with the C−S bond breaking that generates the formylglycine and a CuII-oxyl complex. Moreover, our results suggest that the aldehyde oxygen of the final product originates from O2, which will be useful for future experimental work. 相似文献
85.
Dr. Yusen Li Xi Su Wenhao Zheng Dr. Jia-Jia Zheng Linshuo Guo Prof. Mischa Bonn Prof. Xingfa Gao Dr. Hai I. Wang Prof. Long Chen 《Angewandte Chemie (International ed. in English)》2023,62(10):e202216795
Targeted synthesis of kagome ( kgm ) topologic 2D covalent organic frameworks remains challenging, presumably due to the severe dependence on building units and synthetic conditions. Herein, two isomeric “two-in-one” monomers with different lengths of substituted arms based on naphthalene core (p-Naph and m-Naph) are elaborately designed and utilized for the defined synthesis of isomeric kgm Naph-COFs. The two isomeric frameworks exhibit splendid crystallinity and showcase the same chemical composition and topologic structure with, however, different pore channels. Interestingly, C60 is able to uniformly be encapsulated into the triangle channels of m-Naph-COF via in situ incorporation method, while not the isomeric p-Naph-COF, likely due to the different pore structures of the two isomeric COFs. The resulting stable C60@m-Naph-COF composite exhibits much higher photoconductivity than the m-Naph-COF owing to charge transfer between the conjugated skeletons and C60 guests. 相似文献
86.
Xiuxiu Zhang Chenyu Yang Chen Gong Meihuan Liu Wanlin Zhou Hui Su Feifan Yu Fengchun Hu Qinghua Liu Shiqiang Wei 《Angewandte Chemie (International ed. in English)》2023,62(33):e202308082
Synthesis of highly active and durable oxygen evolution reaction (OER) catalysts applied in acidic water electrolysis remains a grand challenge. Here, we construct a type of high-loading iridium single atom catalysts with tunable d-band holes character (h-HL−Ir SACs, ∼17.2 wt % Ir) realized in the early OER operation stages. The in situ X-ray absorption spectroscopy reveals that the quantity of the d-band holes of Ir active sites can be fast increased by 0.56 unit from the open circuit to a low working potential of 1.35 V. More remarkably, in situ synchrotron infrared and Raman spectroscopies demonstrate the quick accumulation of *OOH and *OH intermediates over holes-modulated Ir sites in the early reaction voltages, achieving a rapid OER kinetics. As a result, this well-designed h-HL−Ir SACs exhibits superior performance for acidic OER with overpotentials of 216 mV @10 mA cm−2 and 259 mV @100 mA cm−2, corresponding to a small Tafel slope of 43 mV dec−1. The activity of catalyst shows no evident attenuation after 60 h operation in acidic environment. This work provides some useful hints for the design of superior acidic OER catalysts. 相似文献
87.
Yang Su Xinlu Wang Minghang Zhang Huimin Guo Prof. Haizhu Sun Gang Huang Prof. Dongtao Liu Prof. Guangshan Zhu 《Angewandte Chemie (International ed. in English)》2023,62(45):e202308182
Zn-I2 batteries have attracted attention due to their low cost, safety, and environmental friendliness. However, their performance is still limited by the irreversible growth of Zn dendrites, hydrogen evolution reactions, corrosion, and shuttle effect of polyiodide. In this work, we have prepared a new porous polymer (CD-Si) by nucleophilic reaction of β-cyclodextrin with SiCl4, and CD-Si is applied to the solid polymer electrolyte (denoted PEO/PVDF/CD-Si) to solve above-mentioned problems. Through the anchoring of the CD-Si, a conductive network with dual transmission channels was successfully constructed. Due to the non-covalent anchoring effect, the ionic conductivity of the solid polymer electrolytes (SPE) can reach 1.64×10−3 S cm−1 at 25 °C. The assembled symmetrical batteries can achieve highly reversible dendrite-free galvanizing/stripping (stable cycling for 7500 h at 5 mA cm−2 and 1200 h at 20 mA cm−2). The solid-state Zn-I2 battery shows an ultra-long life of over 35,000 cycles at 2 A g−1. Molecular dynamics simulations are performed to elucidate the working mechanism of CD-Si in the polymer matrix. This work provides a novel strategy towards solid electrolytes for Zn-I2 batteries. 相似文献
88.
Jiahui Xian Suisheng Li Hui Su Peisen Liao Shihan Wang Yawei Zhang Wenqian Yang Jun Yang Yamei Sun Yaling Jia Qinglin Liu Prof. Qinghua Liu Prof. Guangqin Li 《Angewandte Chemie (International ed. in English)》2023,62(26):e202304007
How to transfer industrial exhaust gases of nitrogen oxides into high-values product is significantly important and challenging. Herein, we demonstrate an innovative method for artificial synthesis of essential α-amino acids from nitric oxide (NO) by reacting with α-keto acids through electrocatalytic process with atomically dispersed Fe supported on N-doped carbon matrix (AD-Fe/NC) as the catalyst. A yield of valine with 32.1 μmol mgcat−1 is delivered at −0.6 V vs. reversible hydrogen electrode, corresponding a selectivity of 11.3 %. In situ X-ray absorption fine structure and synchrotron radiation infrared spectroscopy analyses show that NO as nitrogen source converted to hydroxylamine that promptly nucleophilic attacked on the electrophilic carbon center of α-keto acid to form oxime and subsequent reductive hydrogenation occurred on the way to amino acid. Over 6 kinds of α-amino acids have been successfully synthesized and gaseous nitrogen source can be also replaced by liquid nitrogen source (NO3−). Our findings not only provide a creative method for converting nitrogen oxides into high-valued products, which is of epoch-making significance towards artificial synthesis of amino acids, but also benefit in deploying near-zero-emission technologies for global environmental and economic development. 相似文献
89.
Dr. Junning Kou Dr. Qi Wu Dr. Dongxu Cui Dr. Yun Geng Dr. Kunhao Zhang Prof. Dr. Min Zhang Prof. Dr. Hongying Zang Prof. Dr. Xinlong Wang Prof. Dr. Zhongmin Su Prof. Dr. Chunyi Sun 《Angewandte Chemie (International ed. in English)》2023,62(47):e202312733
Chiral induction has been an important topic in chemistry, not only for its relevance in understanding the mysterious phenomenon of spontaneous symmetry breaking in nature but also due to its critical implications in medicine and the chiral industry. The induced chirality of fullerenes by host–guest interactions has been rarely reported, mainly attributed to their chiral resistance from high symmetry and challenges in their accessibility. Herein, we report two new pairs of chiral porous aromatic cages (PAC), R- PAC-2 , S- PAC-2 (with Br substituents) and R- PAC-3 , S- PAC-3 (with CH3 substituents) enantiomers. PAC-2 , rather than PAC-3 , achieves fullerene encapsulation and selective binding of C70 over C60 in fullerene carbon soot. More significantly, the occurrence of chiral induction between R- PAC-2 , S- PAC-2 and fullerenes is confirmed by single-crystal X-ray diffraction and the intense CD signal within the absorption region of fullerenes. DFT calculations reveal the contribution of electrostatic effects originating from face-to-face arene-fullerene interactions dominate C70 selectivity and elucidate the substituent effect on fullerene encapsulation. The disturbance from the differential interactions between fullerene and surrounding chiral cages on the intrinsic highly symmetric electronic structure of fullerene could be the primary reason accounting for the induced chirality of fullerene. 相似文献
90.
Xi Su Zhiye Zhong Dr. Xiaoli Yan Dr. Ting Zhang Chuanzhe Wang Dr. Yi-Xuan Wang Prof. Gang Xu Prof. Long Chen 《Angewandte Chemie (International ed. in English)》2023,62(22):e202302645
As an emerging class of promising porous materials, the development of two-dimensional conductive metal organic frameworks (2D c-MOFs) is hampered by the few categories and tedious synthesis of the specific ligands. Herein, we developed a nonplanar hexahydroxyl-functionalized Salphen ligand (6OH-Salphen) through a facile two-step synthesis, which was further applied to construct layered 2D c-MOFs through in situ one pot synthesis based on the synergistic metal binding effect of the N2O2 pocket of Salphen. Interestingly, the C2v-symmetry of ligand endows Cu-Salphen-MOF with periodically heterogeneous pore structures. Benefitting from the higher metal density and shorter in-plane metal-metal distance, Cu-Salphen-MOF showcased excellent NO2 sensing performance with good sensitivity, selectivity and reversibility. The current work opens up a new avenue to construct 2D c-MOF directly from nonplanar ligands, which greatly simplifies the synthesis and provides new possibilities for preparing different topological 2D c-MOF based functional materials. 相似文献