The adsorption of sodium oleate(NaOL)at the microfine hematite/aqueous solution interface was investigated in this paper.Experimental research indicated that negative effects stemmed from the dissolution of the microf...The adsorption of sodium oleate(NaOL)at the microfine hematite/aqueous solution interface was investigated in this paper.Experimental research indicated that negative effects stemmed from the dissolution of the microfine hematite(D50=19.21μm)could be effectively eliminated via the appropriate dosage of NaOL at alkali pH conditions.Solution chemistry calculation and adsorption test results indicated that RCOOand(RCOO)_(2)^(2-) ions were responsible for microfine hematite flotation at pH 8.2.Zeta potential and FTIR measurements confirmed the co-adsorption of molecular and ionic oleate species occurred at pH 8.2.X-ray photoelectron spectroscopy(XPS)results further indicated that oleate species interacted with hematite surfaces mainly through chemisorption,giving rise to molecule/colloid formation of oleate and Fe―OL complex compound.Time-of-flight secondary ion mass spectrometry(ToF-SIMS)results demonstrated that oleate species adsorbed onto the hematite surfaces with a thickness of a few nanometers.Furthermore,the normalized peak intensity of C4H7+ions on the hematite sample at pH 8.2 increased remarkably comparing with corresponding result of hematite sample at pH 6.8.The new findings of the present study well revealed the dissolution of microfine hematite and the pH effects on the hematite flotation,as well as the adsorption characteristics of oleate species.展开更多
To ensure a long-term quantum computational advantage,the quantum hardware should be upgraded to withstand the competition of continuously improved classical algorithms and hardwares.Here,we demonstrate a superconduct...To ensure a long-term quantum computational advantage,the quantum hardware should be upgraded to withstand the competition of continuously improved classical algorithms and hardwares.Here,we demonstrate a superconducting quantum computing systems Zuchongzhi 2.1,which has 66 qubits in a two-dimensional array in a tunable coupler architecture.The readout fidelity of Zuchongzhi 2.1 is considerably improved to an average of 97.74%.The more powerful quantum processor enables us to achieve larger-scale random quantum circuit sampling,with a system scale of up to 60 qubits and 24 cycles,and fidelity of FXEB=(3·66±0·345)×10^(-4).The achieved sampling task is about 6 orders of magnitude more difficult than that of Sycamore[Nature 574,505(2019)]in the classic simulation,and 3 orders of magnitude more difficult than the sampling task on Zuchongzhi 2.0[arXiv:2106.14734(2021)].The time consumption of classically simulating random circuit sampling experiment using state-of-the-art classical algorithm and supercomputer is extended to tens of thousands of years(about 4·8×104years),while Zuchongzhi 2.1 only takes about 4.2 h,thereby significantly enhancing the quantum computational advantage.展开更多
Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conducto...Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.展开更多
A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutrali...A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutralization reaction between Cu(OH)_(2)and Nafion in aqueous solution induces the exposing of vast anions which can exclude the in-situ-formed hydroxides and raise the local basicity.Remarkably,the optimal Nafionactivated Cu(OH)_(2)-derived Cu can efficiently suppress the hydrogen evolution reaction(HER)and improve the selectivity for multi-carbon products in the CO_(2)electroreduction reaction(eCO_(2)RR).The H2 Faradaic efficiency(FE)decreased to 11%at a current density of 300 mA/cm2(−0.76 V vs.RHE)in a flow cell,while the bare one with H2 had an FE of 40%.The total eCO_(2)RR FE reaches as high as 83%,along with an evidently increased C2H4 FE of 44%as compared with the bare one(24%),and good stability(8000 s),surpassing that of most of the reported Cu(OH)_(2)-derived Cu.The experimental and theoretical results both show that the strong hydrophobicity and high local basicity jointly boosted the eCO_(2)RR as acquired by felicitously introducing ionomer on the Cu(OH)_(2)-derived Cu surface.展开更多
Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for inc...Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for incorporating high-valence metal ions(Ti^(4+),Sn^(4+),and Zr^(4+))into ultrasmall Fe_(2)O_(3)on carbon nanotube support(i.e.,M-FeO-CNT).The resulting materials exhibit not only a boosted Na+adsorption as shown by density functional theory(DFT)calculations,but also display an increased oxygen deficiency.The electrochemical activity and charge transfer efficiency of Fe 2 O 3 can be improved by reasonably sub-stituting Fe 3+with Ti^(4+),Sn^(4+),and Zr^(4+).The electrochemical investigation of Ti-doped Fe 2 O 3(Ti-FeO-CNT)electrode demonstrates a splendid specific capacitance of 1.25 F cm^(−2)at 1 mA cm^(−2)in 1 M Na_(2)SO_(4).This is significantly higher as compared to the capacitance of 0.48 F cm^(−2).Flexible solid-state asymmetric su-percapacitor Ti-FeO-CNT//MnO_(2)is verified with operating voltage of 2.0 V and stability over 3000 cycles,and delivers a high energy density of 2.14 mWh cm^(−3)at power density of 25 mW cm−3.The flame synthesis is expected to be widely applicable for the preparation of high-valence metal ions doped nanosized Fe_(2)O_(3)functionalized materials,thus opening up new avenues for energy and catalysis research.展开更多
Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impac...Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impact on the adsorption properties. In this study, a novel acidic ionic liquid, 1-butyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfate(i.e., [BTPIm][HSO_4]), was synthesized and subsequently grafted onto the MCM-36 zeolite for the regulation of its adsorption properties towards isobutane and 1-butene. The resultant [BTPIm][HSO_4]-immobilized MCM-36(i.e., MCM-36-IL) was characterized by FT-IR, XPS, XRD, SEM, TG/DTG and N_2 adsorption–desorption measurement. It was found that the specific surface area, micropore volume and mesopore volume of the MCM-36 support underwent a reduction upon the immobilization of ionic liquid,while the surface density of acid increased from 0.0014 to 0.0035 mmol·m^(-2). The adsorption capacity of isobutane and 1-butene on the MCM-36-IL was determined by a static volumetric method. Results demonstrated that the interaction between isobutane and MCM-36-IL was enhanced and the interaction between 1-butene and MCM-36-IL was reduced. As a result, a tunable adsorption ratio of isobutane/1-butene on MCM-36 was achieved.With the increase in surface density of acid and the tunable adsorption ratio of isobutane and 1-butene on the functionalized MCM-36, the acidic ionic liquid-immobilized zeolites are beneficial to obtain an improved reaction yield and a prolonged catalyst life in the reactions catalyzed by solid acid.展开更多
Conversion of CO2 into CO using plasma processing powered by renewable energy is a promising method to convert intermittent sustainable electricity into storable chemical energy.Despite extensive research efforts worl...Conversion of CO2 into CO using plasma processing powered by renewable energy is a promising method to convert intermittent sustainable electricity into storable chemical energy.Despite extensive research efforts worldwide,there is currently no process that achieves economically viable values for both CO2 conversion fraction and energy recovery efficiency simultaneously.Here we demonstrate that a process that utilizes the Boudouard reaction,CO^2++C→2 CO,driven by a thermal plasma allows both 95%CO2 conversion to CO and energy recovery efficiency of 70%,values far higher than seen so far.By comparing the conversion process with and without CO2 excitation by a plasma and by using optical emission spectroscopy we show that the improved performance is due to a novel mode of operation where CO2 is pyrolyzed into an active mixture of CO,O and O2 by an arc discharge which is then introduced into a fixed bed to interact with carbon material.In this way,the free oxygen in the mixture combusts with carbon to form CO,and residual plasma excited CO2 is reduced by carbon.In the overall process,the endothermic Boudouard reaction is partially replaced by an exothermic reaction,and the excess electric energy to produce CO2 plasma is reused in the carbon bed.展开更多
The Histograms of Oriented Gradients(HOG)can produce good results in an image target recognition mission,but it requires the same size of the target images for classification of inputs.In response to this shortcoming,...The Histograms of Oriented Gradients(HOG)can produce good results in an image target recognition mission,but it requires the same size of the target images for classification of inputs.In response to this shortcoming,this paper performs spatial pyramid segmentation on target images of any size,gets the pixel size of each image block dynamically,and further calculates and normalizes the gradient of the oriented feature of each block region in each image layer.The new feature is called the Histogram of Spatial Pyramid Oriented Gradients(HSPOG).This approach can obtain stable vectors for images of any size,and increase the target detection rate in the image recognition process significantly.Finally,the article verifies the algorithm using VOC2012 image data and compares the effect of HOG.展开更多
基金supported by the Natural Science Foundation of China (No. 52164021)the Natural Science Foundation of Yunnan Province (No. 2019FB078)
文摘The adsorption of sodium oleate(NaOL)at the microfine hematite/aqueous solution interface was investigated in this paper.Experimental research indicated that negative effects stemmed from the dissolution of the microfine hematite(D50=19.21μm)could be effectively eliminated via the appropriate dosage of NaOL at alkali pH conditions.Solution chemistry calculation and adsorption test results indicated that RCOOand(RCOO)_(2)^(2-) ions were responsible for microfine hematite flotation at pH 8.2.Zeta potential and FTIR measurements confirmed the co-adsorption of molecular and ionic oleate species occurred at pH 8.2.X-ray photoelectron spectroscopy(XPS)results further indicated that oleate species interacted with hematite surfaces mainly through chemisorption,giving rise to molecule/colloid formation of oleate and Fe―OL complex compound.Time-of-flight secondary ion mass spectrometry(ToF-SIMS)results demonstrated that oleate species adsorbed onto the hematite surfaces with a thickness of a few nanometers.Furthermore,the normalized peak intensity of C4H7+ions on the hematite sample at pH 8.2 increased remarkably comparing with corresponding result of hematite sample at pH 6.8.The new findings of the present study well revealed the dissolution of microfine hematite and the pH effects on the hematite flotation,as well as the adsorption characteristics of oleate species.
基金the National Key R&D Program of China(2017YFA0304300),the Chinese Academy of Sciences,Anhui Initiative in Quantum Information Technologies,Technology Committee of Shanghai Municipality,National Natural Science Foundation of China(11905217,11774326,and 11905294)‘Shang-hai Municipal Science and Technology Major Project(2019SHZDZX01)’Natural Science Foundation of Shanghai(19ZR1462700)‘Key-Area Research and Development Program of Guangdong Province(2020B0303030001)’the Youth Talent Lifting Project(2020-JCJQ-QT-030)。
文摘To ensure a long-term quantum computational advantage,the quantum hardware should be upgraded to withstand the competition of continuously improved classical algorithms and hardwares.Here,we demonstrate a superconducting quantum computing systems Zuchongzhi 2.1,which has 66 qubits in a two-dimensional array in a tunable coupler architecture.The readout fidelity of Zuchongzhi 2.1 is considerably improved to an average of 97.74%.The more powerful quantum processor enables us to achieve larger-scale random quantum circuit sampling,with a system scale of up to 60 qubits and 24 cycles,and fidelity of FXEB=(3·66±0·345)×10^(-4).The achieved sampling task is about 6 orders of magnitude more difficult than that of Sycamore[Nature 574,505(2019)]in the classic simulation,and 3 orders of magnitude more difficult than the sampling task on Zuchongzhi 2.0[arXiv:2106.14734(2021)].The time consumption of classically simulating random circuit sampling experiment using state-of-the-art classical algorithm and supercomputer is extended to tens of thousands of years(about 4·8×104years),while Zuchongzhi 2.1 only takes about 4.2 h,thereby significantly enhancing the quantum computational advantage.
基金supported by the National Natural Science Foundation of China(Nos.52122511,61927814,and U20A20290)Anhui Provincial Natural Science Foundation(2308085QF218)+5 种基金China National Postdoctoral Program for Innovative Talents(BX20230351)China Postdoctoral Science Foundation(2023M733382)National Key R&D Program of China(2021YFF0502700)Major Scientific and Technological Projects in Anhui Province(202203a05020014)Fundamental Research Funds for the Central Universities(WK5290000003 and WK2090000058)Youth Innovation Promotion Association CAS(Y2021118)。
文摘Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.
基金National Natural Science Foundation of China,Grant/Award Numbers:52201227,21972126,51872209,52072273Zhejiang Provincial Special Support Program for High-level Talents,Grant/Award Number:2019R52042Key Project of Zhejiang Provincial Natural Science Foundation,Grant/Award Number:LZ20B030001。
文摘A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutralization reaction between Cu(OH)_(2)and Nafion in aqueous solution induces the exposing of vast anions which can exclude the in-situ-formed hydroxides and raise the local basicity.Remarkably,the optimal Nafionactivated Cu(OH)_(2)-derived Cu can efficiently suppress the hydrogen evolution reaction(HER)and improve the selectivity for multi-carbon products in the CO_(2)electroreduction reaction(eCO_(2)RR).The H2 Faradaic efficiency(FE)decreased to 11%at a current density of 300 mA/cm2(−0.76 V vs.RHE)in a flow cell,while the bare one with H2 had an FE of 40%.The total eCO_(2)RR FE reaches as high as 83%,along with an evidently increased C2H4 FE of 44%as compared with the bare one(24%),and good stability(8000 s),surpassing that of most of the reported Cu(OH)_(2)-derived Cu.The experimental and theoretical results both show that the strong hydrophobicity and high local basicity jointly boosted the eCO_(2)RR as acquired by felicitously introducing ionomer on the Cu(OH)_(2)-derived Cu surface.
基金supported by the National Natu-ral Science Foundation of China(No.21978182)the Miaozi Project in Science and Technology Innovation Program of Sichuan Province(No.21-YCG021).
文摘Doping is a reasonable solution to improve the electronic structure and surface properties of nanomaterials.Herein,we propose a rapid and simple methodology,flame synthesis,as an effective preparation strategy for incorporating high-valence metal ions(Ti^(4+),Sn^(4+),and Zr^(4+))into ultrasmall Fe_(2)O_(3)on carbon nanotube support(i.e.,M-FeO-CNT).The resulting materials exhibit not only a boosted Na+adsorption as shown by density functional theory(DFT)calculations,but also display an increased oxygen deficiency.The electrochemical activity and charge transfer efficiency of Fe 2 O 3 can be improved by reasonably sub-stituting Fe 3+with Ti^(4+),Sn^(4+),and Zr^(4+).The electrochemical investigation of Ti-doped Fe 2 O 3(Ti-FeO-CNT)electrode demonstrates a splendid specific capacitance of 1.25 F cm^(−2)at 1 mA cm^(−2)in 1 M Na_(2)SO_(4).This is significantly higher as compared to the capacitance of 0.48 F cm^(−2).Flexible solid-state asymmetric su-percapacitor Ti-FeO-CNT//MnO_(2)is verified with operating voltage of 2.0 V and stability over 3000 cycles,and delivers a high energy density of 2.14 mWh cm^(−3)at power density of 25 mW cm−3.The flame synthesis is expected to be widely applicable for the preparation of high-valence metal ions doped nanosized Fe_(2)O_(3)functionalized materials,thus opening up new avenues for energy and catalysis research.
基金Supported by the National Natural Science Foundation of China(No.21276163,and No.21576168)
文摘Adsorption properties of an adsorbent or a catalyst towards adsorbates are crucial in the process of adsorption separation or catalytic reaction. Surface morphology and structure of adsorbents have a significant impact on the adsorption properties. In this study, a novel acidic ionic liquid, 1-butyl-3-(triethoxysilylpropyl)imidazolium hydrogen sulfate(i.e., [BTPIm][HSO_4]), was synthesized and subsequently grafted onto the MCM-36 zeolite for the regulation of its adsorption properties towards isobutane and 1-butene. The resultant [BTPIm][HSO_4]-immobilized MCM-36(i.e., MCM-36-IL) was characterized by FT-IR, XPS, XRD, SEM, TG/DTG and N_2 adsorption–desorption measurement. It was found that the specific surface area, micropore volume and mesopore volume of the MCM-36 support underwent a reduction upon the immobilization of ionic liquid,while the surface density of acid increased from 0.0014 to 0.0035 mmol·m^(-2). The adsorption capacity of isobutane and 1-butene on the MCM-36-IL was determined by a static volumetric method. Results demonstrated that the interaction between isobutane and MCM-36-IL was enhanced and the interaction between 1-butene and MCM-36-IL was reduced. As a result, a tunable adsorption ratio of isobutane/1-butene on MCM-36 was achieved.With the increase in surface density of acid and the tunable adsorption ratio of isobutane and 1-butene on the functionalized MCM-36, the acidic ionic liquid-immobilized zeolites are beneficial to obtain an improved reaction yield and a prolonged catalyst life in the reactions catalyzed by solid acid.
基金supported by the National Natural Science Foundation of China(Grants nos.11775155,51561135013,21603202)。
文摘Conversion of CO2 into CO using plasma processing powered by renewable energy is a promising method to convert intermittent sustainable electricity into storable chemical energy.Despite extensive research efforts worldwide,there is currently no process that achieves economically viable values for both CO2 conversion fraction and energy recovery efficiency simultaneously.Here we demonstrate that a process that utilizes the Boudouard reaction,CO^2++C→2 CO,driven by a thermal plasma allows both 95%CO2 conversion to CO and energy recovery efficiency of 70%,values far higher than seen so far.By comparing the conversion process with and without CO2 excitation by a plasma and by using optical emission spectroscopy we show that the improved performance is due to a novel mode of operation where CO2 is pyrolyzed into an active mixture of CO,O and O2 by an arc discharge which is then introduced into a fixed bed to interact with carbon material.In this way,the free oxygen in the mixture combusts with carbon to form CO,and residual plasma excited CO2 is reduced by carbon.In the overall process,the endothermic Boudouard reaction is partially replaced by an exothermic reaction,and the excess electric energy to produce CO2 plasma is reused in the carbon bed.
基金partly supported by the National Natural Science Foundation of China(No.51802348)。
文摘The Histograms of Oriented Gradients(HOG)can produce good results in an image target recognition mission,but it requires the same size of the target images for classification of inputs.In response to this shortcoming,this paper performs spatial pyramid segmentation on target images of any size,gets the pixel size of each image block dynamically,and further calculates and normalizes the gradient of the oriented feature of each block region in each image layer.The new feature is called the Histogram of Spatial Pyramid Oriented Gradients(HSPOG).This approach can obtain stable vectors for images of any size,and increase the target detection rate in the image recognition process significantly.Finally,the article verifies the algorithm using VOC2012 image data and compares the effect of HOG.
