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| 1 | Fe atoms anchored on defective nitrogen doped hollow carbon spheres as efficient electrocatalysts for oxygen reduction reaction显示文摘Defective electrocatalysts,especially for intrinsic defective carbon,have aroused a wide concern owing to high spin and charge densities.However,the designated nitrogen species favorable for creating defects by the removal of nitrogen,and the influence of defects for the coordination structure of active site and oxygen reduction reaction(ORR)activity have not been elucidated.Herein,we designed and synthesized a pair of electrocatalysts,denoted as Fe-N/C and Fe-ND/C for coordination sites of atomic iron-nitrogen and iron-nitrogen/defect configuration embedded in hollow carbon spheres,respectively,through direct pyrolysis of their corresponding hollow carbon spheres adsorbed with Fe(acac)3.The nitrogen defects were fabricated via the evaporation of pyrrolic-N on nitrogen doped hollow carbon spheres.Results of comparative experiments between Fe-N/C and Fe-ND/C reveal that Fe-ND/C shows superior ORR activity with an onset potential of 30 mV higher than that of Fe-N/C.Fe-ND sites are more favorable for the enhancement of ORR activity.Density functional theory(DFT)calculation demonstrates that Fe-ND/C with proposed coordination structure of FeN_(4-x)(0 | Panpan Su Wenjuan Huang Jiangwei Zhang Utsab Guharoy Qinggang Du Qiao Sun Qike Jiang Yi Cheng Jie Yang Xiaoli Zhang Yongsheng Liu San Ping Jiang Jian Liu | 2021 | Nano Research2021,14,4: | 2 |
| 2 | Reactant enrichment in hollow void of Pt NPs@MnOx nanoreactors for boosting hydrogenation performance显示文摘In confined mesoscopic spaces,the unraveling of a catalytic mechanism with complex mass transfer and adsorption processes such as reactant enrichment is a great challenge.In this study,a hollow nanoarchitecture of MnOx-encapsulated Pt nanoparticles was designed as a nanoreactor to investigate the reactant enrichment in a mesoscopic hollow void.By employing advanced characterization techniques,we found that the reactant-enrichment behavior is derived from directional diffusion of the reactant driven through the local concentration gradient and this increased the amount of reactant.Combining experimental results with density functional theory calculations,the superior cinnamyl alcohol(COL)selectivity originates from the selective adsorption of cinnamaldehyde(CAL)and the rapid formation and desorption of COL in the MnOx shell.The superb performance of 95%CAL conversion and 95%COL selectivity is obtained at only 0.5 MPa H2 and 40 min.Our findings showcase that a rationally designed nanoreactor co uld boost catalytic performance in chemoselective hydrogenation,which can be of great aid and potential in various application scenarios. | Yanfu Ma Liwei Wang Wantong Zhao Tianyi Liu Haitao Li Wenhao Luo Qike Jiang Wei Liu Qihua Yang Jun Huang Riguang Zhang Jian Liu GQMax Lu Can Li | 2023 | National Science Review2023,10,10: | 0 |
| 3 | Sub-nanometer Pt_(2)In_(3) intermetallics as ultra-stable catalyst for propane dehydrogenation显示文摘Pt-based catalysts are the typical industrial catalysts for propane dehydrogenation(PDH),which still suffer from insufficient lo ng-term durability due to the structu ral instability and coke deposition.A commercial γ-Al_(2)O_(3) supported thermally robust sub-nanometer Pt2In3intermetallic catalyst with atomically ordered structure and rigorously separated Pt single atoms was fabricated,which showed outstanding robustness in 240 h long-term operation at 600℃ with the deactivation rate constant kdas low as0.00078 h^(-1), ranking among the lowest reported values.Based on various in situ characterizations and theoretical calculations,it was proved that the catalyst stability not only resulted from the separated Pt single-atom sites but also significantly affected by the distance of adjacent Pt atoms.An increasing distance to 3.25 A in the Pt_(2)In_(3)could induce a weak π-adsorption configuration of propylene on Pt sites,which facilitated the desorption of propylene and restrained the side reactions like coking. | Yanan Xing Guiyue Bi Xiaoli Pan Qike Jiang Yuanlong Tan Yang Su Leilei Kang Bonan Li Lin Li Aiqin Wang Jingyuan Ma Xiaofeng Yang Xiao Yan Liu Tao Zhang | 2023 | Journal of Energy Chemistry2023,,8: | 0 |
| 4 | Exhumation and Preservation of the Jinchuan Ni-Cu-PGE Deposit under the East Longshou Mountain Thermal Evolution,Revealed by Apatite Fission Track Thermochronology显示文摘Uplift and exhumation are important factors affecting the preservation of deposits.The anatomy of uplift-cooling evolution and exhumation in the East Longshou Mountain is of significant research value in understanding changes in the Jinchuan Ni-Cu-PGE deposit since its formation.This study uses apatite fission track(AFT)thermochronology to reconstruct the thermal history of the East Longshou Mountain,including the Jinchuan mine,revealing the uplift and exhumation history of the East Longshou Mountain and elucidating the preservation status of the Jinchuan deposit.The AFT ages in the East Longshou Mountain are distributed from 62.3±3.0 Ma to 214.7±14 Ma,with significant differences in ages in distinct areas,the central and pooled ages being consistent within the margin of error.Inverse thermal history models reveal two rapid cooling events associated with exhumation from the Early Jurassic to the Early Cretaceous(200–100 Ma)and since the Miocene(15–0 Ma),the former attributable to the far-afield response to the closure of the PaleoTethys Ocean and plate assembly at the southern margin of Eurasia,the latter associated with the initial India-Eurasia plate collision.A slow cooling event from the Early Cretaceous to the Miocene(100–15 Ma)is thought to be related to the arid environment in northwest China since the Cretaceous.These cooling events have diverse responses and cooling rates in different blocks of the East Longshou Mountain:the southwest and centre of which are mainly cooled over 200–120 Ma and 120–0 Ma,with cooling rates of~0.25 and~0.33°C/Ma(~1.25 and~0.33°C/Ma in the centre);the Jinchuan mine primarily cooled over 160–100 Ma,100–15 Ma and 15–0 Ma,with cooling rates of~1.33,~0.25 and~2.00°C/Ma.These differentiated coolings imply that the uplift of the East Longshou Mountain before the Miocene(~15 Ma)was integral.Strong uplift then occurred in the vicinity of the mining area,which is a critical period for the uplift of the Jinchuan deposit to the surface,meaning that the Jinchuan deposit was exposed no earlier than the Miocene(~15 Ma).Based on mineralization depth information obtained by previous researchers,in conjunction with the calculation and simulation results of this study,it can be seen that the bulk of the Jinchuan intrusion may still be preserved at depth. | LEI Xianghe YU Qiang JIAO Jiangang LIU Jian SUN Xianyao HE Lijuan YANG Qike | 2023 | Acta Geologica Sinica(English Edition)2023,97,2: | 0 |
| 5 | Boosting CO_(2) electroreduction to formate via bismuth oxide clusters显示文摘Supported metal(oxide)clusters,with both rich surface sites and high atom utilization efficiency,have shown improved activity and selectivity for many catalytic reactions over nanoparticle and single atom catalysts.Yet,the role of cluster catalysts has been rarely reported in CO_(2)electroreduction reaction(CO_(2)RR),which is a promising route for converting CO_(2)to liquid fuels like formic acid with renewable electricity.Here we develop a bismuth oxide(BiOn)cluster catalyst for highly efficient CO_(2)RR to formate.The BiOn cluster catalyst exhibits excellent activity,selectivity,and stability towards formate production,with a formate Faradaic efficiency of over 90%at a current density up to 500 mA·cm^(−2)in an alkaline membrane electrode assembly electrolyzer,corresponding to a mass activity as high as 3,750 A·gBi−1.The electrolyzer with the BiOn cluster catalyst delivers a remarkable formate production rate of 0.56 mmol·min−1 at a high single-pass CO_(2)conversion of 44%.Density functional theory calculations indicate that Bi4O_(3)cluster is more favorable for stabilizing the HCOO^(*)intermediate than Bi(001)surface and single site BiC_(4)motif,rationalizing the improved formate production over the BiOn cluster catalyst.This work highlights the great importance of cluster catalysts in activity and selectivity control in electrocatalytic CO_(2)conversion. | Xiaole Jiang Le Lin Youwen Rong Rongtan Li Qike Jiang Yaoyue Yang Dunfeng Gao | 2023 | Nano Research2023,16,10: | 0 |
| 6 | Characteristics and evolution of faults in the north-central Yin’e Basin and the effects on the coal-seam in the Cretaceous strata显示文摘Research on the characteristics of faults and their evolutionary history since the Cretaceous in the Suhongtu-Dagu depressions can provide a theoretical basis for geological evaluation of the coal seams in the Suhongtu Formation in the northern-central region of the Yin’e Basin.Using 3-D seismic-logging inversion techniques,seismic stratigraphic calibration,stratigraphic sequence delineation,and thickness calculations on the Suhongtu-Dagu depressions were carried out to clarify the planar and profile distributions of the faults,as well as the evolutionary history of these faults and the tectonic history of the depressions.The results of this study revealed that the distribution of the faults in the Suhongtu-Dagu depressions in the northern part of the Yin’e Basin varies with region,and the fault system was multi-period,orthotropic,north-east-trending,and north-north-east-trending,with a certain degree of inheritance in terms of the geological setting.Three types of faults were identified:Y-shaped fractures,reverse Y-shaped fractures,and parallel fractures,which can be classified as Paleozoic-Cenozoic continuous syncline faults and intra-depression faults from the top of the Permian to the Upper Cretaceous series and inter-stratigraphic adjustment faults within the Cretaceous System,respectively.The evolution of these faults can be divided into three phases:the controlling faults were the faults that existed before the Early Cretaceous and had been active since then;synclinal faults that formed during the Early Cretaceous;and modified faults that formed since the Early Cretaceous.The development and modification of the coal seams in the Cretaceous Suhongtu Formation in the Hari,Kuanzihu,and Babei sags were strongly controlled and influenced by a multi-phase complex fault system. | Qiang YU Baojiang WANG Zhanli REN Xianyao SUN Xianghe LEI Ahmed KHALED Qike YANG | 2023 | Frontiers of Earth Science2023,17,1: | 0 |