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1.
Proc Natl Acad Sci U S A ; 119(8)2022 02 22.
Article in English | MEDLINE | ID: mdl-35169079

ABSTRACT

The onset of mountain building along margins of the Tibetan Plateau provides a key constraint on the processes by which the high topography in Eurasia formed. Although progressive expansion of thickened crust underpins most models, several studies suggest that the northern extent of the plateau was established early, soon after the collision between India and Eurasia at ca. 50 Ma. This inference relies heavily on the age and provenance of Cenozoic sediments preserved in the Qaidam basin. Here, we present evidence in the northern plateau for a considerably younger inception and evolution of the Qaidam basin, based on magnetostratigraphies combined with detrital apatite fission-track ages that date the basin fills to be from ca. 30 to 4.8 Ma. Detrital zircon-provenance analyses coupled with paleocurrents reveal that two-stage growth of the Qilian Shan in the northeastern margin of the Tibetan Plateau began at ca. 30 and at 10 Ma, respectively. Evidence for ca. 30 and 10 to 15 Ma widespread synchronous deformation throughout the Tibetan Plateau and its margins suggests that these two stages of outward growth may have resulted from the removal of mantle lithosphere beneath different portions of the Tibetan Plateau.

2.
iScience ; 24(2): 102109, 2021 Feb 19.
Article in English | MEDLINE | ID: mdl-33615204

ABSTRACT

Photocatalytic transformation of biomass into value-added chemicals coupled with co-production of hydrogen provides an explicit route to trap sunlight into the chemical bonds. Here, we demonstrate a rational design of Zn1-xCdxS solid solution homojunction photocatalyst with a pseudo-periodic cubic zinc blende (ZB) and hexagonal wurtzite (WZ) structure for efficient glucose conversion to simultaneously produce hydrogen and lactic acid. The optimized Zn0.6Cd0.4S catalyst consists of a twinning superlattice, has a tuned bandgap, and displays excellent efficiency with respect to hydrogen generation (690 ± 27.6 µmol·h-1·gcat. -1), glucose conversion (~90%), and lactic acid selectivity (~87%) without any co-catalyst under visible light irradiation. The periodic WZ/ZB phase in twinning superlattice facilitates better charge separation, while superoxide radical (⋅O2 -) and photogenerated holes drive the glucose transformation and water oxidation reactions, respectively. This work demonstrates that rational photocatalyst design could realize an efficient and concomitant production of hydrogen and value-added chemicals from glucose photocatalysis.

3.
Chem Commun (Camb) ; 56(13): 1944-1947, 2020 Feb 13.
Article in English | MEDLINE | ID: mdl-31967625

ABSTRACT

The lack of efficient hydrogen storage material is one of the bottlenecks for the large-scale implementation of hydrogen energy. Here, a series of new hydrogen storage materials, i.e., anilinide-cyclohexylamide pairs, are proposed via the metallation of an aniline-cyclohexylamine pair. DFT calculations show that the enthalpy change of hydrogen desorption (ΔHd) can be significantly tuned from 60.0 kJ per mol-H2 for the pristine aniline-cyclohexylamine pair to 42.2 kJ per mol-H2 for sodium anilinide-cyclohexylamide and 38.7 kJ per mol-H2 for potassium anilinide-cyclohexylamide, where an interesting correlation between the electronegativity of the metal and the ΔHd was observed. Experimentally, the sodium anilinide-cyclohexylamide pair was successfully synthesised with a theoretical hydrogen capacity of 4.9 wt%, and the hydrogenation and dehydrogenation cycle can be achieved at a relatively low temperature of 150 °C in the presence of commercial catalysts, in clear contrast to the pristine aniline-cyclohexylamine pair which undergoes dehydrogenation at elevated temperatures.

4.
Nat Commun ; 8: 15887, 2017 06 21.
Article in English | MEDLINE | ID: mdl-28635970

ABSTRACT

The appearance of detritus shed from mountain ranges along the northern margin of the Tibetan Plateau heralds the Cenozoic development of high topography. Current estimates of the age of the basal conglomerate in the Qaidam basin place this event in Paleocene-Eocene. Here we present new magnetostratigraphy and mammalian biostratigraphy that refine the onset of basin fill to ∼25.5 Myr and reveal that sediment accumulated continuously until ∼4.8 Myr. Sediment provenance implies a sustained source in the East Kunlun Shan throughout this time period. However, the appearance of detritus from the Qilian Shan at ∼12 Myr suggests emergence of topography north of the Qaidam occurred during the late Miocene. Our results imply that deformation and mountain building significantly post-date Indo-Asian collision and challenge the suggestion that the extent of the plateau has remained constant through time. Rather, our results require expansion of high topography during the past 25 Myr.

6.
Sci Rep ; 6: 29568, 2016 07 14.
Article in English | MEDLINE | ID: mdl-27411593

ABSTRACT

Significant climate shifts in the northeastern Tibetan Plateau have taken place during the Cenozoic, but the reasons behind them remain unclear. In order to unravel the mechanisms driving these climate changes, proxy data with accurate age constraint are needed. Here we present magnetostratigraphy, sediment color (redness a*, and lightness L*) and grain-size analysis from an early to middle Miocene (~20-15.3 Ma) sediment sequence preserved in the Yumen Basin on the northeastern Tibetan Plateau. In this basin, remarkable increase in lightness, decreases in redness and in ratio of hematite (Hm) to goethite (Gt) took place at ~16.5 Ma. We suggest that these changes result from shorter duration of weathering, climatic wetting, and cooling associated with rapid uplift of the Qilian Shan at the middle Miocene.

7.
Sci Rep ; 6: 27604, 2016 06 09.
Article in English | MEDLINE | ID: mdl-27277834

ABSTRACT

The Cenozoic basins and ranges form the high topography of the northeastern Tibet that resulted from the India-Eurasia collision. Sedimentary rocks in the basins provide direct insight into the exhumation history of the ranges and the tectonic processes that led to the northeastward growth of the Tibetan Plateau. In this study, we analyzed and compared detrital zircon U-Pb ages from sands of modern rivers draining the Bei Shan, and North Qilian Shan and sandstones from the Yumen Basin. The zircon age distributions indicate that the strata dated to 24.2-16.7 Ma in the basin were derived from the Bei Shan, and the basin provenance changed rapidly to the North Qilian Shan terrane at ~16 Ma. These results suggest that an early stage of deformation along the Bei Shan at ~24 Ma was replaced by the growth of the North Qilian Shan at ~16 Ma. We conclude that the far-field effect associated with the Indo-Asian collision may result from Oligocene deformation in the Bei Shan, but the emergence of the North Qilian Shan at ~16 Ma could reflect the most recent outward growth of the Tibetan Plateau that may have been caused by the removal of some lithospheric mantle beneath central Tibet.

8.
Inorg Chem ; 54(4): 1556-62, 2015 Feb 16.
Article in English | MEDLINE | ID: mdl-25642733

ABSTRACT

Pure BaMgSiO4:Eu(2+) phosphor, prepared by a solid state reaction method under N2 atmosphere, exhibited a strong green emission at 500 nm and a weak emission at 405 nm. Heat treatment under NH3 atmosphere causes changes in the PL intensity: the green emission at 500 nm gradually decreases and completely disappears after heat treatment for 3 h, whereas a new blue emission peak, centered at 445 nm, appears and becomes very strong. The results of the analyses with electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine structure (XAFS) spectroscopy suggest that the heat treatment causes the generation of a large amount of oxygen vacancies. This resulted in the aforementioned color changes of the BaMgSiO4:Eu phosphor, which are confirmed by the results of DFT+U calculations. In particular, these calculations showed that Eu prefers to occupy Ba(3) sites, which are six coordinated to oxygen atoms. The emission at 500 nm was attributed to the 4f-5d transition energy of Eu in Ba(3) site, calculated as 2.54 eV. It was also shown that Eu 4f energy level decreases when oxygen is removed from the oxygen position adjacent to Eu, which results in a larger Eu 4f-5d transition energy and shorter wavelengths of emission peaks.

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