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981.
Guo-Qiang Tang Xian-Hua Li Qiu-Li Li Yu Liu Xiao-Xiao Ling 《Surface and interface analysis : SIA》2020,52(5):190-196
Carbonate oxygen (O) and carbon (C) isotopes are widely used as proxies for tracing the processes and physicochemical conditions of many geological events and environmental changes in Earth Science. In particular, O and C isotopic variations at micrometer scales revealed by modern microbeam analytical techniques such as SIMS and NanoSIMS are robust archives for reconstructing palaeoenvironment and paleoclimate changes at annual and seasonal resolution or even higher temporal resolution. Widespread application of carbonate O and C isotopic microanalysis in Earth Sciences, however, has been restricted due to limitation of high-quality carbonate reference materials for O and C isotopic microanalysis. We introduce in this paper a new calcite reference material for calcite O and C isotopic microanalysis. This calcite is collected from a drill-core of the Oka carbonatite complex (Quebec, Canada). We demonstrated that the Oka calcite is fairly homogeneous in O and C isotopic compositions at micrometer scales based on homogeneity test by hundreds of SIMS O and C isotopic analyses. Precise determinations by using conventional gas-source IRMS yield the recommended value of δ18OVPDB = −23.12 ± 0.15‰ (1SD) and δ13CVPDB = −5.23 ± 0.06‰ (1SD) for the Oka calcite, which has been certified as the first class of Chinese national certified reference material (GBW04481) for O and C isotopic microanalysis. 相似文献
982.
Taylor D. Krueger Dr. Longteng Tang Dr. Liangdong Zhu Isabella L. Breen Prof. Dr. Rebekka M. Wachter Prof. Dr. Chong Fang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(4):1661-1669
The molecular mechanisms for the photoconversion of fluorescent proteins remain elusive owing to the challenges of monitoring chromophore structural dynamics during the light-induced processes. We implemented time-resolved electronic and stimulated Raman spectroscopies to reveal two hidden species of an engineered ancestral GFP-like protein LEA, involving semi-trapped protonated and trapped deprotonated chromophores en route to photoconversion in pH 7.9 buffer. A new dual-illumination approach was examined, using 400 and 505 nm light simultaneously to achieve faster conversion and higher color contrast. Substitution of UV irradiation with visible light benefits bioimaging, while the spectral benchmark of a trapped chromophore with characteristic ring twisting and bridge-H bending motions enables rational design of functional proteins. With the improved H-bonding network and structural motions, the photoexcited chromophore could increase the photoswitching-aided photoconversion while reducing trapped species. 相似文献
983.
Kwanghak Choe Fengbin Zheng Dr. Hui Wang Yi Yuan Wenshi Zhao Dr. Guangxin Xue Xueying Qiu Myonghak Ri Prof. Xinghua Shi Prof. Yinglong Wang Prof. Guodong Li Prof. Zhiyong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3679-3686
The semihydrogenation of alkynes into alkenes rather than alkanes is of great importance in the chemical industry. Unfortunately, state-of-the-art heterogeneous catalysts hardly achieve high turnover frequencies (TOFs) simultaneously with almost full conversion, excellent selectivity, and good stability. Here, we used metal–organic frameworks (MOFs) containing Zr metal nodes (“UiO”) with tunable wettability and electron-withdrawing ability as activity accelerators for the semihydrogenation of alkynes catalyzed by sandwiched palladium nanoparticles (Pd NPs). Impressively, the porous hydrophobic UiO support not only leads to an enrichment of phenylacetylene around the Pd NPs but also renders the Pd surfaces more electron-deficient, which leads to a remarkable catalysis performance, including an exceptionally high TOF of 13835 h−1, 100 % phenylacetylene conversion 93.1 % selectivity towards styrene, and no activity decay after successive catalytic cycles. The strategy of using molecularly tailored supports is universal for boosting the selective semihydrogenation of various terminal and internal alkynes. 相似文献
984.
Chaohai Wang Dr. Jeonghun Kim Dr. Jing Tang Dr. Jongbeom Na Prof. Yong-Mook Kang Minjun Kim Hyunsoo Lim Prof. Yoshio Bando Prof. Jiansheng Li Prof. Yusuke Yamauchi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(5):2082-2086
Carbon aerogels (CAs) with 3D interconnected networks hold promise for application in areas such as pollutant treatment, energy storage, and electrocatalysis. In spite of this, it remains challenging to synthesize high-performance CAs on a large scale in a simple and sustainable manner. We report an eco-friendly method for the scalable synthesis of ultralight and superporous CAs by using cheap and widely available agarose (AG) biomass as the carbon precursor. Zeolitic imidazolate framework-8 (ZIF-8) with high porosity is introduced into the AG aerogels to increase the specific surface area and enable heteroatom doping. After pyrolysis under inert atmosphere, the ZIF-8/AG-derived nitrogen-doped CAs show a highly interconnected porous mazelike structure with a low density of 24 mg cm−3, a high specific surface area of 516 m2 g−1, and a large pore volume of 0.58 cm−3 g−1. The resulting CAs exhibit significant potential for application in the adsorption of organic pollutants. 相似文献
985.
Prof. Shuaijun Yang Ping-An Yin Lin Li Prof. Qian Peng Prof. Xinggui Gu Prof. Ge Gao Prof. Jingsong You Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(25):10222-10228
Squaraines (SQs) with tunable emission in the solid state is of great importance for various demands; however a remaining challenge is emission quenching upon aggregation. Herein, a unique SQ, named as CIEE-SQ, is designed to exhibit strong emission in crystal, undergoing crystallization-induced reverse from dark 1(n+σ,π*) to bright 1(π,π*) excited states. Such an excited state of CIEE-SQ can be subtly tuned by molecular conformation changes during the unexpected temperature-triggered single-crystal to single-crystal (SCSC) reversible transformation. Furthermore, co-crystallization between CIEE-SQ and chloroform largely stabilize the 1(π,π*) state, enhancing the transition dipole moment and decreasing the reorganization energy to boost the fluorescence, which is promising in data encryption and decryption. 相似文献
986.
Celina Love Jan Steinkühler David T. Gonzales Naresh Yandrapalli Tom Robinson Rumiana Dimova Dr. T.-Y. Dora Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(15):6006-6013
In situ, reversible coacervate formation within lipid vesicles represents a key step in the development of responsive synthetic cellular models. Herein, we exploit the pH responsiveness of a polycation above and below its pKa, to drive liquid–liquid phase separation, to form single coacervate droplets within lipid vesicles. The process is completely reversible as coacervate droplets can be disassembled by increasing the pH above the pKa. We further show that pH-triggered coacervation in the presence of low concentrations of enzymes activates dormant enzyme reactions by increasing the local concentration within the coacervate droplets and changing the local environment around the enzyme. In conclusion, this work establishes a tunable, pH responsive, enzymatically active multi-compartment synthetic cell. The system is readily transferred into microfluidics, making it a robust model for addressing general questions in biology, such as the role of phase separation and its effect on enzymatic reactions using a bottom-up synthetic biology approach. 相似文献
987.
Tzu-Yu Chen Jinfeng Chen Yijie Tang Dr. Jiahai Zhou Dr. Yisong Guo Dr. Wei-chen Chang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(19):7437-7441
N-alkylisonitrile, a precursor to isonitrile-containing lipopeptides, is biosynthesized by decarboxylation-assisted -N≡C group (isonitrile) formation by using N-alkylglycine as the substrate. This reaction is catalyzed by iron(II) and 2-oxoglutarate (Fe/2OG) dependent enzymes. Distinct from typical oxygenation or halogenation reactions catalyzed by this class of enzymes, installation of the isonitrile group represents a novel reaction type for Fe/2OG enzymes that involves a four-electron oxidative process. Reported here is a plausible mechanism of three Fe/2OG enzymes, Sav607, ScoE and SfaA, which catalyze isonitrile formation. The X-ray structures of iron-loaded ScoE in complex with its substrate and the intermediate, along with biochemical and biophysical data reveal that -N≡C bond formation involves two cycles of Fe/2OG enzyme catalysis. The reaction starts with an FeIV-oxo-catalyzed hydroxylation. It is likely followed by decarboxylation-assisted desaturation to complete isonitrile installation. 相似文献
988.
Wei Zhou Jun-Kang Guo Sheng Shen Jinbo Pan Jie Tang Lang Chen Chak-Tong Au Shuang-Feng Yin 《物理化学学报》2020,36(3):1906048-0
CO_2是最常见的化合物,作为潜在的碳一资源,可用于制备多种高附加值的化学品,如一氧化碳、甲烷、甲醇、甲酸等。传统的热催化转化CO_2方法能耗高,反应条件苛刻。因此,如何在温和条件下高效地将CO_2转化成高附加值的化学品,一直以来是催化领域的研究热点和难点之一。光催化技术反应条件温和、绿色环保。然而,纯光催化反应普遍存在太阳能利用效率有限,光生载流子分离效率低等问题。针对上述问题,在光催化的基础上引入电催化,可以提高载流子的分离效率,在较低的过电位下,实现多电子、质子向CO_2转移,从而提高催化反应效率。总之,光电催化技术可以结合光催化和电催化的优势,提高CO_2催化还原反应效率,为清洁、绿色利用CO_2提供了一种新方法。本文依据光电催化CO_2还原反应基本过程,从光吸收、载流子分离和界面反应等三个角度综述了光电催化反应的基本强化策略,并对未来可能的研究方向进行了展望。 相似文献
989.
Zian Tang Dr. Antony George Dr. Andreas Winter David Kaiser Christof Neumann Dr. Thomas Weimann Prof. Dr. Andrey Turchanin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6473-6478
Field effect transistors (FETs) based on 2D materials are of great interest for applications in ultrathin electronic and sensing devices. Here we demonstrate the possibility to add optical switchability to graphene FETs (GFET) by functionalizing the graphene channel with optically switchable azobenzene molecules. The azobenzene molecules were incorporated to the GFET channel by building a van der Waals heterostructure with a carbon nanomembrane (CNM), which is used as a molecular interposer to attach the azobenzene molecules. Under exposure with 365 nm and 455 nm light, azobenzene molecules transition between cis and trans molecular conformations, respectively, resulting in a switching of the molecular dipole moment. Thus, the effective electric field acting on the GFET channel is tuned by optical stimulation and the carrier density is modulated. 相似文献
990.
采用水热法并经氨气保护热处理制备了双过渡金属氮化物Co3W3N/CNTs复合材料,得到了价格低廉且拥有良好氮电化学还原性能(NRR)的催化剂。通过调节已经预氧化的CNTs与过渡金属氮化物前驱体CoWO4的比例以及氨气热处理温度,实现了Co3W3N在CNTs表面的均匀负载。扫描电子显微镜(SEM)及透射电子显微镜(TEM)测试结果显示该电化学活性纳米微粒均匀地分散于CNTs表面,表明经预氧化的CNTs由于表面富集了较多的活性基团,有利于双过渡金属氮化物的分散生长。热处理后CNTs表面的Co3W3N微粒尺寸约为20 nm,相较于无载体的Co3W3N尺寸(100 nm)有明显减小。室温条件下,在N2饱和的0.01 mol·L^-1 H2SO4溶液中测试了该纳米复合材料在不同过电位下的NRR,该材料在-0.3 V(vs RHE)时的产氨率及法拉第效率分别可达12.73μg·h^-1·cm-2和13.59%,对比同样条件下,纯相Co3W3N的产氨率及法拉第效率仅为1.08μg·h^-1·cm^-2和1.76%。结果表明,通过水热反应和氨气保护热处理的Co3W3N/CNTs纳米复合材料具有良好的NRR性能。 相似文献