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Nickel-modified In_(2)O_(3) with inherent oxygen vacancies for CO_(2) hydrogenation to methanol

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Science China Chemistry 2024年第5期67卷 1715-1728页

作者： Zixuan Zhou Yuchen Wang Yuanjie Bao Haiyan Yang Jiong Li Chunran Chang Shenggang Li Peng Gao CAS Key Laboratory of Low-carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

Methanol synthesis is one of the most important industrially-viable approaches for carbon dioxide(CO_(2)) utilization, as the produced methanol can be used as a platform chemical for manufacturing green fuels and chemicals. The In_(2)O_(3) catalysts are ideal for sustainable methanol synthesis and have received considerable attention. Herein, Co-, Ni-and Cu-modified In_(2)O_(3) catalysts were fabricated with high dispersion and high stability to improve the hydrogenation performance. The Ni-promoted In_(2)O_(3) catalyst in the form of high dispersion possessed the largest amount of oxygen vacancies and the strongest ability for H_(2) activation, leading to the highest CO_(2) conversion and space time yield of methanol of 0.390 g_(Me OH)g_(cat)^(-1)h^(-1) with CH_(3)OH selectivity of 68.7%. In addition, the catalyst exhibits very stable performance over 120 h on stream, which suggests the promising prospect for industrial applications. Further experimental and theoretical studies demonstrate that surface Ni doping promotes the formation of oxygen defects on the In_(2)O_(3) catalyst, although it also results in lower methanol selectivity. Surprisingly, subsurface Ni dopants are found to be more beneficial for methanol formation than surface Ni dopants, so the Nipromoted In_(2)O_(3)catalyst with a lower surface Ni content at the similar Ni loading can reach higher methanol selectivity and productivity. This work thus provides theoretical guidance for significantly improving the CO_(2) reactivity of In_(2)O_(3)-based catalysts while maintaining high methanol selectivity.

关键词： carbon dioxide hydrogenation methanol synthesis indium oxides Ni doping sites transition metal promoters

Mechanisms behind the environmental sensitivity of carbon fiber reinforced polytetrafluoroethylene(PTFE)

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Friction 2024年第5期12卷 997-1015页

作者： Pontus JOHANSSON P.MARKLUND M.BJORLING Y.SHI division of Machine Element LuleåUniversity of TechnologyLuleåSE-97187Sweden

carbon fiber reinforced polytetrafluoroethylene (CF/PTFE) composites are known for their exceptional tribological performance when sliding against steel or cast iron in inert gas environments. Compared to experiments in humid air, about an order of magnitude lower wear rate and several times lower coefficient of friction have been reported for tests conducted in dry nitrogen and hydrogen. Moreover, trace moisture has been shown to affect the friction and wear significantly of this tribosystem, although a possible effect of oxygen cannot be ruled out due to uncertainties regarding the oxygen concentrations. While several studies have pointed out the environmental sensitivity of CF/PTFE, the understanding of the underlying mechanisms are very limited. The objective of this research is to investigate the individual and combined effect of oxygen and moisture on the tribological behavior of CF/PTFE sliding against steel. Additionally, this study aims to elucidate the underlying mechanisms that govern the environmental sensitivity of the system. Climate-controlled three-pin-on-disc experiments were conducted in nitrogen atmospheres at various concentrations of oxygen and moisture. The tribological results clearly demonstrate that both moisture and oxygen contribute to increased friction and wear. However, the adverse effect was much more pronounced for oxygen than moisture. A qualitative method was developed to estimate the tribofilm coverage on the CF/PTFE surface. Results showed strong correlation between high coverage of strongly adhered tribofilm and low wear rate. Moreover, a loosely adhered tribofilm was observed on top of the CF/PTFE surface in presence of moisture. FTIR analysis indicated that the loosely adhered tribofilm found in the moisture-enriched environment contained a significant amount of adsorbed water, which may explain the lower coefficient of friction in presence of moisture compared to oxygen. The adsorbed water in the loosely adhered tribofilm coul

关键词： polymer composite tribofilm tribochemistry atmosphere

Exploring pore-scale production characteristics of oil shale after CO_(2) huff‘n’puff in fractured shale with varied permeability

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International Journal of Coal Science & Technology 2024年第1期11卷 194-203页

作者： Tianhan Xu Jian Wang Yuhao Lu Danling Wang Li Yu Ye Tian State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum UniversityChengdu610500SichuanChina Institute for carbon Neutrality Southwest Petroleum UniversityChengdu610500SichuanChina research Institute of Shenzhen Branch of CNOOC(China)Co. LtdShenzhen518000GuangdongChina PetroChina Huabei Oilfield Company Cangzhou062552HebeiChina

Recent studies have indicated that the injection of carbon dioxide(CO_(2))can lead to increased oil recovery in fractured shale reservoirs following natural *** advancements in understanding mass exchange processes in subsurface formations,there remains a knowledge gap concerning the disparities in these processes between the matrix and fractures at the pore scale in formations with varying *** study aims to experimentally investigate the CO_(2) diffusion behaviors and in situ oil recovery through a CO_(2) huff‘n’puff process in the Jimsar shale oil *** achieve this,we designed three matrix-fracture models with different permeabilities(0.074 mD,0.170 mD,and 0.466 mD)and experimented at 30 MPa and 91℃.The oil concentration in both the matrix and fracture was monitored using a low-field nuclear magnetic resonance(LF-NMR)technique to quantify in situ oil recovery and elucidate mass-exchange *** results showed that after three cycles of CO_(2) huff‘n’puff,the total recovery degree increased from 30.28%to 34.95%as the matrix permeability of the core samples increased from 0.074 to 0.466 mD,indicating a positive correlation between CO_(2) extraction efficiency and matrix *** similar fracture conditions,the increase in matrix permeability further promoted CO_(2) extraction efficiency during CO_(2) huff‘n’***,the increase in matrix permeability of the core had the greatest effect on the extraction of the first-cycle injection in large pores,which increased from 16.42%to 36.64%.The findings from our research provide valuable insights into the CO_(2) huff‘n’puff effects in different pore sizes following fracturing under varying permeability conditions,shedding light on the mechanisms of CO_(2)-enhanced oil recovery in fractured shale oil reservoirs.

关键词： Shale reservoir Hydraulic fracturing CO_(2)huff‘n’puff NMR Production characteristics

Bamboo-derived hard carbon/carbon nanotube composites as anode material for long-life sodium-ion batteries with high charge/discharge capacities

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Rare Metals 2024年第1期43卷 124-137页

作者： Sukanya Pothaya Chatwarin Poochai Nantikan Tammanoon Yaowamarn Chuminjak Tanaporn Kongthong Tanom Lomas Chakrit Sriprachuabwong Adisorn Tuantranont Graphene and Printed Electronics for Dual-Use Applications research division(GPERD) National Security and Dual-Use Technology Center(NSD)National Science and Technology Development Agency(NSTDA)Tambon Klong NuengAmphoe Klong LuangPathum Thani 12120Thailand

Hard carbon derived from bamboo for the anode material of sodium-ion batteries has a three-dimensional(3D) open framework structure and has naturally incorporated K-ions into its carbon structure,increasing the dinterlayer spacing of hard carbon materials for facilitating Na^(+) *** this work,bamboo-derived hard carbon was prepared via two carbonization temperatures at 700and 1000 ℃ for an hour and employed as an anode for sodium-ion batteries(SIB).X-ray diffraction(XRD) and Fourier transform(FT)-Raman spectroscopic results indicated the disordered structure with d-spacing(d_(002)) around0.36-0.37 nm,which is a benefit for sodium ion insertion/***,the composition between carbon-nanotube(CNT) and bamboo-derived hard carbon(BB) was synthesized by a ball mill with various contents of CNT(1 wt%,5 wt% and 10 wt%).At the optimal CNT content of 5 wt%,the sample exhibited excellent performance and outstanding *** the anode,the half-cell SIB using BB(700)w@5%CNT(with a carbonization temperature of700 ℃ and CNT loading of 5 wt%) delivered a high initial specific capacity of 268.9 mAh·g^(-1) at 0.1C and capacity retention of 78.6% after 500 cycles at *** full cell SIB fabrication BB(700)w@5%CNT in combination with Na_(3)V_(2)(PO4)_(3) as the cathode demonstrated a high specific capacity of 127.6 mAh·g^(-1) at 0.2C with its capacitive retention remaining of 78% at 1.0C after 1000 *** attained storage performance indicates that hard carbonCNT composite anode material enhanced the conductive path of electron transport and provided long-term cycling *** good electrochemical performance as well as the low cost and environment-friendliness of the bambooderived hard carbon proves its suitability for future sodium-ion batteries.

关键词： Hard carbon Bamboo Sodium-ion battery(SIB) Full cell

Characteristics of super drought in Southwest China and the associated compounding effect of multiscalar anomalies

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Science China Earth Sciences 2024年第7期67卷 2084-2102页

作者： Lin WANG Wen CHEN Gang HAUNG Ting WANG Qiulin WANG Xiaoyun SU Zixuan REN Chakrit CHOTAMONSAK Atsamon LIMSAKUL Kritanai TORSRI CAS Key Laboratory of Regional Climate-Environment for Temperate East Asia Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Heavy Rain and Drought-Flood Disasters in Plateau and Basin Key Laboratory of Sichuan Province Chengdu 610072China Department of Atmospheric Science Yunnan UniversityKunming 650500China State Key Laboratory of Numerical Modeling for Atmospheric Sciences and Geophysical Fluid Dynamics Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China carbon Neutrality research Center Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Hangzhou Meteorological Bureau Hangzhou 310051China Center for Monsoon System research Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Department of Geography Faculty of Social SciencesChiang Mai UniversityChiang Mai 50200Thailand Environmental Science research Center Faculty of ScienceChiang Mai UniversityChiang Mai 50200Thailand Climate Change and Environmental research Center TechnopolisKlong 5Klong LuangPathumthani 12120Thailand Hydro-Informatics Innovation division Hydro-Informatics InstituteMinistry of Higher EducationScienceResearch and InnovationBangkok 10900Thailand

In recent decades,Southwest China(SWC)has suffered from frequent super droughts,leading to severe economic losses and ecological *** study investigates the characteristics of super droughts in SWC during 1961-2022,reveals the compounding effect of multiscalar anomalies,and explores the plausible atmospheric circulation mechanisms *** nature of super drought is a compound drought caused by the superposition of extreme drought events across multiple time *** contrasting the typical drought cases in 2006 and 2022,the decisive role of multiscalar drought compounding is *** on the Comprehensive Multiscalar Index(CMI),multiple super drought events in SWC were identified to be temporally clustered during *** them,the decadal background of enhanced evaporation and precipitation deficit at long time scales is a necessary condition for shaping the overall pattern of super droughts,while the precipitation and evaporation anomalies at short time scales trigger the outbreak of super droughts,determining the exact timing of *** events include August-September 2006,November 2009 to May 2010,July-October 2011,April-May 2012,January-April 2013,*** results suggest that the contribution of superposed precipitation anomalies to super drought is 2.4 times that of *** regards the circulation mechanisms affecting multiscalar precipitation,the anomalous spatial patterns at short-term and long-term scales are similar,featuring the cyclonic circulation over the South China Sea and the northeasterly wind anomalies together with the subsidence center over *** 2006-2014,the possible causes for the cross-seasonal persistent precipitation reduction in SWC are the extreme negative phase of the Pacific Decadal Oscillation(PDO)in the North Pacific as well as the pronounced warming of the warm pool in the western *** key dynamic processes are outlined as *** the one hand,the negative PDO p

关键词： Super drought Multiscalar Compounding effect Mechanism analysis Southwest China

The dynamic catalysis of Ga/ZSM-5 catalysts for propane-CO_(2) coupling conversion to aromatics and syngas

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Journal of Energy Chemistry 2024年第10期97卷 513-519,I0011页

作者： Yonggui Song Zhong-Pan Hu Haohao Feng Enze Chen Le Lv Yimo Wu Zhen Liu Yong Jiang Xiaozhi Su Feifei Xu Mingchang Zhu Jingfeng Han Yingxu Wei Svetlana Mintova Zhongmin Liu The Key Laboratory of the Inorganic Molecule-Based Chemistry of Liaoning Province and Laboratory of Coordination Chemistry Shenyang University of Chemical TechnologyShenyang110142LiaoningChina National Engineering research Center of Lower-carbon Catalysis Technology Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Shanghai Advanced research Institute Chinese Academy of SciencesShanghai 201203China Normandie University Laboratory of Catalysis and Spectrochemistry(LCS)NSICAENUNICAENCNRSCaen 1450France

Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO_(2) hydrogenation,reverse water-gas shift reaction,and propane-CO_(2) coupling ***,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO_(2) during the propane and CO_(2) coupling *** optimizing the reaction conditions,a notable propane conversion rate of 97.9%and an impressive aromatics selectivity of 80.6%in hydrocarbons can be achieved at the conditions of 550℃and CO_(2)/C_(3)H_(8) of 4.^(13)CO_(2)isotope experiments illustrate that C-atoms of CO_(2) can enter into CO(86.5%)and aromatics(10.8%)during the propane-CO_(2) coupling reaction *** situ XANES and FTIR spectroscopies at 550℃and H_(2)/C_(3)H_(8) atmosphere reveal that GaO_(x) species can be gradually dispersed into[GaH_(2)]^(+)/[GaH]^(2+)on the Bronsted acid sites of ZSM-5 zeolite during H_(2) and/or C_(3)H_(8) treatment,which are the real active sites for propane-CO_(2) coupling *** situ CO_(2)-FTIR experiments demonstrate that the[GaH_(2)]^(+)/[GaH]^(2+)species can react with CO_(2) and accelerate the propane and CO_(2) coupling *** work not only presents a cost-effective avenue for CO_(2) utilization,but also contributes to the active site design for improved alkane and CO_(2) activation in coupling reaction system.

关键词： carbon dioxide Propane aromatization Ga/ZSM-5 Gallium hydride Spectroscopy

Numerical Simulation Study on Influence of Equation of State on Internal Flow Field and Performance of S-CO_(2)Compressor

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Journal of Thermal Science 2024年第3期33卷 888-898页

作者： ZHANG Lei YANG Zhenyu SUN Enhui ZHANG Qian AN Guangyao YUAN Wei Hebei Key Laboratory of Low carbon and High Efficiency Power Generation Technology North China Electric Power UniversityBaoding071003China School of Energy Power&Mechanical EngineeringNorth China Electric Power UniversityBaoding071028China

The low power consumption of the near-critical compressor is the key factor for the high efficiency of supercritical CO_(2)Brayton *** the numerical simulation of the compressor,the rapid changes in the thermophysical properties of the CO_(2)near the critical point make it difficult to capture the condensation *** paper investigates the influence of fluid physical properties on the condensation ***,the differences in the physical properties of CO_(2)in the SRK EOS(equation of state),PR EOS,and SW EOS are ***,the simulation of nozzles and compressors were carried out and *** show that the condensation positions predicted by the three EOSs are basically the *** with SW EOS,the disparities between the maximum condensation mass fraction predicted by the PR and SRK EOSs is5.7%and 11.5%,and that of total pressure ratio is 0.3%and 3.8%,*** results show that PR EOS can be considered for numerical simulation in engineering *** its physical property calculation results are closer to the actual physical properties while the physical properties change more gently,it has considerable accuracy and numerical stability.

关键词： supercritical carbon dioxide equation of state centrifugal compressor numerical simulation condensation

Sulfonated carbon dots modified IrO_(2)nanosheet as durable and high-efficient electrocatalyst for boosting acidic oxygen evolution reaction

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Nano research 2024年第9期17卷 8017-8024页

作者： Mengjie Ma Wenxiang Zhu Fan Liao Kui Yin Hui Huang Kun Feng Dongdong Gao Jinxin Chen Zenan Li Jun Zhong Lai Xu Yang Liu Mingwang Shao Zhenhui Kang Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering(MIMSE) Macao University of Science and TechnologyTaipaMacao 999078China

Oxygen evolution reaction(OER)plays a crucial role in developing energy conversion and adjusting electronic structure of the electrocatalysts can effectively improve the catalytic activity and ***,it is a challenge to adjust the electronic structure on two-dimensional iridium dioxide nanosheets(IrO_(2)NS),which have the advantages of high atom ***,we regulate the surface properties of IrO_(2)NS through sulfonated carbon dots(SCDs)to promote the OER catalytic *** catalyst IrO_(2)NS/SCDs-2 exhibited excellent catalytic activity with a lower overpotential of 180 mV than IrO_(2)NS(230 mV)at the current density of 10 mA·cm^(-2)in a 0.5 M H_(2)SO_(4) *** after 160 h of stability testing,the overpotential of IrO_(2)NS/SCDs-2 only decreased by 4 ***,transient potential scanning test can visually demonstrate that the addition of SCDs improves the conductivity of the catalyst and increases the electron transfer rate.

关键词： sulfonated carbon dots oxygen evolution reaction electrocatalysis transient potential scanning

Flexible printed three dimensional(3D) integrated carbon nanotube complementary metal oxide semiconductor(CMOS) thin film transistors and circuits

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Science China(Information Sciences) 2024年第9期67卷 280-293页

作者： Zhaofeng CHEN Jiaqi LI Min LI Hongxuan GUO Jianwen ZHAO SEU-FEI Nano-Pico Center Key Laboratory of MEMS of Ministry of Education Southeast University Printable Electronics research Center Division of Nanodevices and Related NanomaterialsSuzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences School of Nano Technology and Nano Bionics University of Science and Technology of China

The threshold voltage modulation of carbon nanotube thin-film transistors（TFTs） and flexible three-dimensional（3D） integration circuits has become hot research topics for carbon-based electronics. In this paper, a doping-free gate electrode technology is introduced to significantly modulate the threshold voltage of polymer-sorted semiconducting single-walled carbon nanotube（sc-SWCNT） TFTs in combination with the highly effective gate-controlling ability of solid-state electrolyte thin films as the dielectrics. A systematic investigation was conducted on the impact of printed silver, evaporated silver, and evaporated aluminum（Al） gate electrodes on the threshold voltage of flexible printed bottom-gate and top-gate SWCNT TFTs. The results indicate that the SWCNT TFTs with Al gate electrodes exhibit enhancement-mode characteristics with excellent electrical properties, such as the negative threshold voltages（-0.6 V）, high Ion/Ioff（up to 10～6）, low subthreshold swing(61.4 mV · dec-1), and small hysteresis. It is attributed to either the formation of lower work function thin films（Al2O3） at the electrode/dielectric layer interfaces through the natural oxidation of the Al bottom-gate electrodes or the dipole reaction of the Al top-gate electrodes from X-ray photoelectron spectroscopy（XPS） and ultraviolet photoelectron spectroscopy（UPS） data. In addition, 3D complementary metal-oxide-semiconductor（CMOS） inverters with common gate electrodes were constructed using the resulting enhancement-mode P-type SWCNT TFTs and matched N-type SWCNT TFTs, which shows high voltage gain（34）, rail-to-rail output and high noise margins(80.04%, VDD=-1 V)as well good mechanical flexibility at low operation voltages. It demonstrates that SWCNT TFTs have great advantages for building large-scale 3D flexible integrated circuits.

关键词： three-dimensional CMOS circuits printing technology polymer-sorted semiconducting carbon nanotubes enhancement-mode thin-filmtransistors threshold voltage modulation