Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Multi-metal hydroxides possess unique physical and chemical properties,making them promising candidates for supercapacitor working electrodes.Enhancing their electrochemical performance can be achieved through a combi...Multi-metal hydroxides possess unique physical and chemical properties,making them promising candidates for supercapacitor working electrodes.Enhancing their electrochemical performance can be achieved through a combination with carbon materials.In this study,we synthesized a composite material by hydrothermally dispersed 4,6,and 10 wt%carbon nanotubes(CNT)into ternary cobaltbismuth-samarium hydroxide(CoBiSm-TOH).These nanocomposites were employed as the material for the working electrode in a supercapacitor.The findings reveal that at 1.5 A/g,the specific capacitance of CNT3@CoBiSm-TOH,using a three-electrode system,was found to be 852.91 F/g,higher than that of CoBi-BOH,CoBiSm-TOH,CNT1@CoBiSm-TOH and CNT5@CoBiSm-TOH-measuring 699.69,750.34,789.54 and 817.79 F/g,respectively.Moreover,CNT3@CoBiSm-TOH electrodes exhibited a capacitance retention of around 88%over 10,000 cycles.To demonstrate practical applicability,CNT3@CoBiSm-TOH was grown on woven carbon fiber(WCF),and a solid-state supercapacitor device was developed using the VARTM(vacuum-assisted resin transfer molding).This device displayed a specific capacitance of 272.67 F/g at 2.25 A/g.Notably,it achieved a maximum energy density of 53.01 Wh/kg at a power density of 750 W/kg and sustained excellent cycle stability over 50,000 cycles,maintaining 70%of its initial capacitance.These results underscore the importance of interfacial nanoengineering and provide crucial insights for the development of future energy storage devices.展开更多
This paper presents a study on CO<sub>2</sub> atmospheric transformation which was reacted directly with lithium hydroxide solution and metallic lithium. This solution was obtained through the reaction bet...This paper presents a study on CO<sub>2</sub> atmospheric transformation which was reacted directly with lithium hydroxide solution and metallic lithium. This solution was obtained through the reaction between metallic lithium and deionized water where hydrogen is produced and by exposing the metal at ambient conditions. In the transformation process, atmospheric CO<sub>2</sub> gas reacts directly with LiOH solution, in both cases, the CO<sub>2</sub> transformation kinetics was different. For this purpose, reactions between CO<sub>2</sub> and LiOH solution were carried out under controlled temperature and the second process only with metallic lithium, which was exposed at room temperature, however, in these two processes lithium carbonate oxide was formed and identified. According to the results, the efficiency in CO<sub>2</sub> transformation is a function of temperature value which was variable until completely obtaining the by-product, its XRD characterization indicated the formation only of Li<sub>2</sub>CO<sub>3</sub> in both procedures. Under laboratory conditions lithium compounds selectively reacted with CO<sub>2</sub>. In the same way, there is an alternative procedure to obtain LiOH and Li<sub>2</sub>CO<sub>3</sub> for different applications in various areas.展开更多
Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction...Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.展开更多
Composite solid base catalysts derived from Ca‐M‐Al(M=Mg,La,Ce,Y)layered double hydroxides(LDH)were synthesized,characterized and applied to the transesterification of methanol with propylene carbonate.X‐ray diffra...Composite solid base catalysts derived from Ca‐M‐Al(M=Mg,La,Ce,Y)layered double hydroxides(LDH)were synthesized,characterized and applied to the transesterification of methanol with propylene carbonate.X‐ray diffraction analyses of the catalysts show that all of the catalysts were in the form of composite oxides.Compared with the Ca‐Al LDH catalyst,the specific surface areas and pore volumes of the catalysts were increased with the introduction of Mg,La or Ce.The catalytic performance of these catalysts increases in the order of Ca‐Y‐Al<Ca‐Al<Ca‐Ce‐Al<Ca‐La‐Al<Ca‐Mg‐Al,which is consistent with the total surface basic amounts of these materials and the formation of especially strong basic sites following modification with Mg and La.The Ca‐Mg‐Al catalyst shows the highest(Ca+Mg):Al atomic ratio,indicating that it likely contains more unsaturated O2?ions,providing it with the highest concentration of very strong basic sites.The recyclability of these catalysts is improved following the addition of Mg,La,Ce or Y,with the Ca‐Mg‐Al maintaining a high level of activity after ten recycling trials.X‐ray diffraction analyses of fresh and used Ca‐Mg‐Al demonstrate that this catalyst is exceptionally stable,which could be of value in practical applications related to heterogeneous catalysis.展开更多
Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt ca...Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt carbonate hydroxide nanoarrays(CoxMoyCH) are designed and synthesized as a bifunctional catalyst towards UOR and HER. Benefiting from the Mo doping, the dispersed nanoarray structure and redistributed electron density, the CoxMoyCH catalyst display outstanding catalytic performance and durability for both HER and UOR, affording the overpotential of 82 m V for HER and delivering a low potential of the 1.33 V for UOR(vs. reversible hydrogen electrode, RHE) to attain a current density of 10 m A cm^(-2), respectively. Remarkably, when CoxMoyCH was applied as bifunctional catalyst in a twoelectrode electrolyzer, a working voltage of 1.40 V is needed in urea-assisted water electrolysis at10 m A cm^(-2) and without apparent decline for 40 h, outperforming the working voltage of 1.51 V in conventional water electrolysis.展开更多
Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow ...Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow active materials with promoted reaction reversibility,accelerated kinetic and restricted volume change still remains a huge challenge.Herein,a novel chemical interaction motivated structure design strategy has been proposed,and a chemically bonded Co(CO_(3))_(0.5)OH·0.11 H_(2)O@MXene(CoCH@MXene)layered-composite was fabricated for the first time.In such a composite,the chemical interaction between Co^(2+)and MXene drives the growth of smaller-sized CoCH crystals and the subsequent formation of interwoven CoCH wires sandwiched in-between MXene nanosheets.This unique layered structure not only encourages charge transfer for faster reaction dynamics,but buffers the volume change of CoCH during lithiation-delithiation process,owing to the confined crystal growth between conductive MXene layers with the help of chemical bonding.Besides,the sandwiched interwoven CoCH wires also prevent the stacking of MXene layers,further conducive to the electrochemical performance of the composite.As a result,the as-prepared CoCH@MXene anode demonstrates a high reversible capacity(903.1 mAh g^(-1)at 100 mA g^(-1))and excellent cycling stability(maintains 733.6 mAh g^(-1)at1000 mA g^(-1)after 500 cycles)for lithium ion batteries.This work highlights a novel concept of layerby-layer chemical interaction motivated architecture design for futuristic high performance electrode materials in energy storage systems.展开更多
Even though a lot of research has been carried out concerning the preparation of carbonate apatite (CHA), they were related to CHA in the form of powder. In the present study, macroporous CHA bone substitutes were pre...Even though a lot of research has been carried out concerning the preparation of carbonate apatite (CHA), they were related to CHA in the form of powder. In the present study, macroporous CHA bone substitutes were prepared through composition-transformation of gypsum and Ca-hydroxide. Here, we investigated the effect of added Ca-hydroxide to gypsum, carbonation periods, and hydrothermal temperatures for phosphatization to understand the basic principle of composition-transformation of gypsum added Ca-hydroxide to fabricate CHA bone substitutes. The specimens were characterized in terms of chemical and physical properties, such as extent of transformation of macroporous gypsum added Ca-hydroxide into CHA body, type and content of carbonate, and crystal morphology. It was observed that the transformation was faster with higher hydrothermal temperature. However, higher hydrothermal temperature caused de-carbonation phenomena which resulted in the lack of carbonate ions of the product. Moreover, the higher the percentage of Ca-hydroxide added to gypsum, caused the complete transformation of gypsum into CHA to be slower. These findings have been applied to the standard fabrication procedure of carbonate apatite, which in turn will allow scaling up process, and will be provided for biomedical purposes for the Indonesian community.展开更多
The precursor of ammonium aluminum carbonate hydroxide was synthesized by using aluminum sulfate（Al2（SO4）3） and ammonium carbonate（（NH4）2CO3）. The effects of α-Al2O3 seeds and mixture composed of α-Al2O3 and...The precursor of ammonium aluminum carbonate hydroxide was synthesized by using aluminum sulfate（Al2（SO4）3） and ammonium carbonate（（NH4）2CO3）. The effects of α-Al2O3 seeds and mixture composed of α-Al2O3 and ammonium nitrate, as well as multiplex catalysts （AT） on phase transformation of alumina in sintering process were investigated respectively. The results show that the α-Al2O3 seeds and the mixture of α-Al2O3 and ammonium nitrate can lower the phase transformation temperature of α-Al2O3 to different extents while the particles obtained agglomerate heavily. AT has great potential synergistic effects on the phase transformation of alumina and reduces the phase transformation temperature of α-Al2O3 and the trends of necking-formation between particles. Therefore the dispersion of powder particles is improved significantly.展开更多
Energy density and production cost for high-performance electrode materials are the main challenge for the capacitive storage technology. In this paper, novel Hydroxide Zinc Carbonate (Zn4CO3(OH)6·H2O, HZC) c...Energy density and production cost for high-performance electrode materials are the main challenge for the capacitive storage technology. In this paper, novel Hydroxide Zinc Carbonate (Zn4CO3(OH)6·H2O, HZC) catalyst layers, which are composed of irregular stagger arrangement nanosheets, have been synthesized successfully on foam Ni from inorganic precursors by a feasible in situ hydrothermal method. Measured by electrochemical tests as electrode materials for supercapacitors, the HZC@Ni foam show high specific capacitance (1329.2 F·g−1 at 1 A·g−1 and 882.8 F·g−1 at 10 A·g−1, respectively). These results show that the HZC@Ni foam could be a potential electrode material for supercapacitors. These encouraging results make these low-cost and eco-friendly materials promising for energy storage application.展开更多
Alpha nickel hydroxide has better performances than commercial beta nickel hydroxide. However, the main defect is that α-phase is difficult to synthesize and easily transformed to β-phase Ni（OH）2 upon aging in a s...Alpha nickel hydroxide has better performances than commercial beta nickel hydroxide. However, the main defect is that α-phase is difficult to synthesize and easily transformed to β-phase Ni（OH）2 upon aging in a strong alkaline solution. In this study, the Al-Co, Al-Yb, Yb-Co and Al-Yb-Co multiple doping was used respectively. By controlling the amount of sodium carbonate, the α-Ni（OH）2 was prepared by ultrasonic-assisted precipitation. And the influence of sodium carbonate on the crystalline phase and structure stability for alpha nickel hydroxide was studied. The results demonstrate that, with increasing amount, the biphase nickel hydroxide transforms to pure alpha nickel hydroxide gradually, and the structure stability is also improved. When the amount of sodium carbonate is 2 g, the sample still keeps α-Ni（OH）2 after being aged for 30 days, for Al-Yb-Co-Ni（OH）2. And when the amount is less than 2 g, the phase transformations exist in the samples with different extents. These results demonstrated that the amount of sodium carbonate is a critical factor to maintain the structural stability of α-Ni（OH）2.展开更多
Layered double hydroxides(LDHs)have received extensive attention in many fields such as catalysis,environmental management and medical applications.Typically,expensive soluble metal salts are commonly used as the star...Layered double hydroxides(LDHs)have received extensive attention in many fields such as catalysis,environmental management and medical applications.Typically,expensive soluble metal salts are commonly used as the starting materials for the synthesis of LDHs.Here,we report a novel synthesis route for Mg/Al-LDH by using inexpensive basic magnesium carbonate as the starting material.X-ray diffraction(XRD)and solid-state nuclear magnetic resonance(ssNMR)data show that LDHs with rich defects are formed rapidly at room temperature and good crystallinity can be obtained after further hydrothermal treatment.These results provide a simple,rapid and green preparation method for LDHs.展开更多
A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co（NO3）O2 solutio...A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co（NO3）O2 solution with carbon nanotubes as matrix exhibited large pseudo-capacitance of 322 F/g in 1 mol/L KOH. To characterize the cobalt hydroxide nanocomposite electrode, a charge-discharge cycling test, cyclic voltammetry, and an impedance test were done. This cobalt hydroxide composite exhibiting excellent pseudo-capacitive behavior （i.c. high reversibility, high specific capacitance, low impedance）, was demonstrated to be a candidate for the application of electrochemical supercapacitors. A combined capacitor consisting of cobalt hydroxide composite as a cathode and activated carbon fiber as an anode was reported. The electrochemical pcrformance of the combined capacitor was characterized by cyclic voltammetry and a dc charge/discharge test. The combined capacitor showed ideal capacitor behavior with an extended operating voltage of 1.4 V. According to the extended operating voltage, the energy density of the combined capacitor at a current density of 100 mA/cm^2 was found to be 11 Wh/kg. The combined capacitor exhibited high-energy density and stable power characteristics,展开更多
The increasing importance of the ecologically minded production of building materials makes it necessary to develop reasonable alternatives to the CO2-intense production of ordinary Portland cement （OPC）. The develo...The increasing importance of the ecologically minded production of building materials makes it necessary to develop reasonable alternatives to the CO2-intense production of ordinary Portland cement （OPC）. The development of new or modified concrete is an important part of existing strategies to improve performance and minimize life-cycle costs. Therefore, we investigated carbonation resistance properties of sulphoaluminate cement （SAC） concrete incorporating layered double hydroxides （LDHs）. X-ray diffraction （XRD） and IR-spectroscopy were employed to characterize the component and structural changes of LDHs and cement paste before and after carbonation test. Carbonation resistance of concrete was experimentally evaluated. Finally, carbonation of Portland cement and SAC concrete was compared. The experimental results show that carbonation depth decreases remarkably with the addition of LDHs, especially the calcinated LDHs. Carbonation depth of SAC concrete is smaller than that of PC concrete regardless of curing time.展开更多
A new design route was presented to fabricate cobalt aluminum-layered double hydroxide(CoAl-LDH)thin layers whichgrow on carbon spheres(CSs)through a growth method.The CoAl-LDH thin layers consist of nanoflakes with a...A new design route was presented to fabricate cobalt aluminum-layered double hydroxide(CoAl-LDH)thin layers whichgrow on carbon spheres(CSs)through a growth method.The CoAl-LDH thin layers consist of nanoflakes with a thickness of20nm.The galvanostatic charge-discharge test of the CoAl-LDH/CSs composite shows a great specific capacitance of1198F/g at1A/g(based on the mass of the CoAl-LDH/CSs composite)in6mol/L KOH solution,and the composite displays an impressive specificcapacitance of920F/g even at a high current density of10A/g.Moreover,the composite remains a specific capacitance of928F/gafter1000cycles at2A/g,and the specific capacitance retention is84%,indicating that the composite has high specific capacitance,excellent rate capability and good cycling stability in comparison to pristine CoAl-LDH.展开更多
Mineral carbonation using waste cement is a promising method to solve the problems caused by CO_2 emission and waste cement. Compaction pressure is an important parameter for mineral carbonation of calcium hydroxide, ...Mineral carbonation using waste cement is a promising method to solve the problems caused by CO_2 emission and waste cement. Compaction pressure is an important parameter for mineral carbonation of calcium hydroxide, one of the most dominant composite of waste cement that can be carbonated. The carbonation degree, morphology of products and compressive strength of carbonated compacts are influenced by compaction pressure significantly. Results show that the carbonation degree of calcium hydroxide increases at first（0-8 MPa） and then decreases in the higher compaction pressure range（10-14 MPa）. At the meantime, results also indicate that lower compaction pressure accelerates the early carbonation but hinder carbonation in the later stages. For the morphologies of carbonation products, calcium carbonate tends to form typical crystal morphology of calcite（rhombohedral） under lower compaction pressure, while it will become ellipsoidlike when compaction pressure reaches 8 MPa. TGA and water content results show that there is an optimal water content for the carbonation. In addition, lower water content is adverse to the carbonation at later stage and the CO_2 is difficult to penetrate into the inside of compacts when water content is high, which will hinder the carbonation. XRD and TGA results show that the carbonation products are calcite and small amount of amorphous calcium carbonate.展开更多
The glassy carbon (GC) electrode modified with a monolayer nickel hydroxide (GC/Ni(OH) 2) was prepared by immersion of GC substrate in 1.0×10 -3 mol/L NiSO 4 solution, and then cyclic voltammetric scannin...The glassy carbon (GC) electrode modified with a monolayer nickel hydroxide (GC/Ni(OH) 2) was prepared by immersion of GC substrate in 1.0×10 -3 mol/L NiSO 4 solution, and then cyclic voltammetric scanning in 0.20 mol/L KOH. Similarly, GC/Co(OH) 2 electrode was prepared too. The experiments showed that the voltammetric behavior of GC/Ni(OH) 2 electrode in 0.20 mol/L KOH is more stable than that of GC/ Co(OH) 2. It was found that the GC/Ni(OH) 2 electrode acts as an effective electrocatalysis for the oxidation of hydrazine.展开更多
Nickel hydroxide doped with multi-wall carbon nanotubes(MCNTs)was synthesized by chemical coprecipitation method. The MCNTs doped nickel hydroxide was used as the electrochemical active material in the positive electr...Nickel hydroxide doped with multi-wall carbon nanotubes(MCNTs)was synthesized by chemical coprecipitation method. The MCNTs doped nickel hydroxide was used as the electrochemical active material in the positive electrodes of rechargeable alkaline batteries.The powder X-ray diffraction(XRD)analysis shows that the addition of MCNTs induces more structural defect within the crystal lattice of the nickel hydroxide.The cyclic voltammetry(CV)and electrochemical impedance spectroscopy(EIS) tests demonstrate the better reaction reversibility and lower electrochemical impedance of MCNTs doped nickel hydroxide as compared with the pure nickel hydroxide.The charge/discharge tests show that MCNTs addition can improve the specific discharge capacity and increase the discharge voltage of the nickel hydroxide electrode.展开更多
Ni/Mg/Al layered double hydroxides(LDHs) with different n(Ni)∶n(Mg)∶n(Al) ratio values were prepared via a coprecipitation reaction. Then Ni/Mg/Al mixed oxides were obtained by calcination of these LDHs precursors. ...Ni/Mg/Al layered double hydroxides(LDHs) with different n(Ni)∶n(Mg)∶n(Al) ratio values were prepared via a coprecipitation reaction. Then Ni/Mg/Al mixed oxides were obtained by calcination of these LDHs precursors. Carbon nanotubes were produced in the catalytic decomposition of propane over the Ni/Mg/Al mixed oxide catalysts. The quality of as-made nanotubes was investigated by SEM and TEM. The nanotubes were multiwall with a high length-diameter ratio and appeared to be flexible. The catalytic activities of these mixed oxides increased with increasing the Ni content. The Ni/Mg/Al mixed oxide with the highest Ni content [n(Ni)/n(Mg)/n(Al)=1/1/1] showed the highest activity and the carbon nanotubes grown on its surface had the best quality.展开更多
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金financially supported by 2024 Gyeongbuk Green Environment Support Center。
文摘Multi-metal hydroxides possess unique physical and chemical properties,making them promising candidates for supercapacitor working electrodes.Enhancing their electrochemical performance can be achieved through a combination with carbon materials.In this study,we synthesized a composite material by hydrothermally dispersed 4,6,and 10 wt%carbon nanotubes(CNT)into ternary cobaltbismuth-samarium hydroxide(CoBiSm-TOH).These nanocomposites were employed as the material for the working electrode in a supercapacitor.The findings reveal that at 1.5 A/g,the specific capacitance of CNT3@CoBiSm-TOH,using a three-electrode system,was found to be 852.91 F/g,higher than that of CoBi-BOH,CoBiSm-TOH,CNT1@CoBiSm-TOH and CNT5@CoBiSm-TOH-measuring 699.69,750.34,789.54 and 817.79 F/g,respectively.Moreover,CNT3@CoBiSm-TOH electrodes exhibited a capacitance retention of around 88%over 10,000 cycles.To demonstrate practical applicability,CNT3@CoBiSm-TOH was grown on woven carbon fiber(WCF),and a solid-state supercapacitor device was developed using the VARTM(vacuum-assisted resin transfer molding).This device displayed a specific capacitance of 272.67 F/g at 2.25 A/g.Notably,it achieved a maximum energy density of 53.01 Wh/kg at a power density of 750 W/kg and sustained excellent cycle stability over 50,000 cycles,maintaining 70%of its initial capacitance.These results underscore the importance of interfacial nanoengineering and provide crucial insights for the development of future energy storage devices.
文摘This paper presents a study on CO<sub>2</sub> atmospheric transformation which was reacted directly with lithium hydroxide solution and metallic lithium. This solution was obtained through the reaction between metallic lithium and deionized water where hydrogen is produced and by exposing the metal at ambient conditions. In the transformation process, atmospheric CO<sub>2</sub> gas reacts directly with LiOH solution, in both cases, the CO<sub>2</sub> transformation kinetics was different. For this purpose, reactions between CO<sub>2</sub> and LiOH solution were carried out under controlled temperature and the second process only with metallic lithium, which was exposed at room temperature, however, in these two processes lithium carbonate oxide was formed and identified. According to the results, the efficiency in CO<sub>2</sub> transformation is a function of temperature value which was variable until completely obtaining the by-product, its XRD characterization indicated the formation only of Li<sub>2</sub>CO<sub>3</sub> in both procedures. Under laboratory conditions lithium compounds selectively reacted with CO<sub>2</sub>. In the same way, there is an alternative procedure to obtain LiOH and Li<sub>2</sub>CO<sub>3</sub> for different applications in various areas.
基金financially supported by the National Natural Science Foundation of China(No.52173055 and 21961132024)the Natural Science Foundation of Shanghai(No.19ZR1401100)+3 种基金the International Cooperation Fund of Science and Technology Commission of Shanghai Municipality(No.21130750100)the Innovation Program of Shanghai Municipal Education Commission(No.2017-01-07-00-03-E00024)the Fundamental Research Funds for the Central Universities(No.18D310109)the DHU Distinguished Young Professor Program(No.LZA2020001).
文摘Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.
基金supported by the Natural Science Foundation of Shanxi Province(201601D102006)the Key Science and Technology Program of Shanxi Province,China(MD2014-09,MD2014-10)~~
文摘Composite solid base catalysts derived from Ca‐M‐Al(M=Mg,La,Ce,Y)layered double hydroxides(LDH)were synthesized,characterized and applied to the transesterification of methanol with propylene carbonate.X‐ray diffraction analyses of the catalysts show that all of the catalysts were in the form of composite oxides.Compared with the Ca‐Al LDH catalyst,the specific surface areas and pore volumes of the catalysts were increased with the introduction of Mg,La or Ce.The catalytic performance of these catalysts increases in the order of Ca‐Y‐Al<Ca‐Al<Ca‐Ce‐Al<Ca‐La‐Al<Ca‐Mg‐Al,which is consistent with the total surface basic amounts of these materials and the formation of especially strong basic sites following modification with Mg and La.The Ca‐Mg‐Al catalyst shows the highest(Ca+Mg):Al atomic ratio,indicating that it likely contains more unsaturated O2?ions,providing it with the highest concentration of very strong basic sites.The recyclability of these catalysts is improved following the addition of Mg,La,Ce or Y,with the Ca‐Mg‐Al maintaining a high level of activity after ten recycling trials.X‐ray diffraction analyses of fresh and used Ca‐Mg‐Al demonstrate that this catalyst is exceptionally stable,which could be of value in practical applications related to heterogeneous catalysis.
基金financially supported by the National Natural Science Foundation of China(52025013,22121005)the 111 Project(B12015)+1 种基金Haihe Laboratory of Sustainable Chemical Transformationsthe Fundamental Research Funds for the Central Universities。
文摘Combining urea oxidation reaction(UOR) with hydrogen evolution reaction(HER) is an effective method for energy saving and highly efficient electrocatalytic hydrogen production. Herein, molybdenumincorporated cobalt carbonate hydroxide nanoarrays(CoxMoyCH) are designed and synthesized as a bifunctional catalyst towards UOR and HER. Benefiting from the Mo doping, the dispersed nanoarray structure and redistributed electron density, the CoxMoyCH catalyst display outstanding catalytic performance and durability for both HER and UOR, affording the overpotential of 82 m V for HER and delivering a low potential of the 1.33 V for UOR(vs. reversible hydrogen electrode, RHE) to attain a current density of 10 m A cm^(-2), respectively. Remarkably, when CoxMoyCH was applied as bifunctional catalyst in a twoelectrode electrolyzer, a working voltage of 1.40 V is needed in urea-assisted water electrolysis at10 m A cm^(-2) and without apparent decline for 40 h, outperforming the working voltage of 1.51 V in conventional water electrolysis.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.51673123 and No.22005346)the National Key R&D Program of China(No.2017YFE0111500)+1 种基金the State Key Laboratory of Polymer Materials Engineering(Grant No.:sklpme2020-1-02)Financial support provided by the Fundamental Research Funds for the Central Universities(No.YJ202118)。
文摘Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow active materials with promoted reaction reversibility,accelerated kinetic and restricted volume change still remains a huge challenge.Herein,a novel chemical interaction motivated structure design strategy has been proposed,and a chemically bonded Co(CO_(3))_(0.5)OH·0.11 H_(2)O@MXene(CoCH@MXene)layered-composite was fabricated for the first time.In such a composite,the chemical interaction between Co^(2+)and MXene drives the growth of smaller-sized CoCH crystals and the subsequent formation of interwoven CoCH wires sandwiched in-between MXene nanosheets.This unique layered structure not only encourages charge transfer for faster reaction dynamics,but buffers the volume change of CoCH during lithiation-delithiation process,owing to the confined crystal growth between conductive MXene layers with the help of chemical bonding.Besides,the sandwiched interwoven CoCH wires also prevent the stacking of MXene layers,further conducive to the electrochemical performance of the composite.As a result,the as-prepared CoCH@MXene anode demonstrates a high reversible capacity(903.1 mAh g^(-1)at 100 mA g^(-1))and excellent cycling stability(maintains 733.6 mAh g^(-1)at1000 mA g^(-1)after 500 cycles)for lithium ion batteries.This work highlights a novel concept of layerby-layer chemical interaction motivated architecture design for futuristic high performance electrode materials in energy storage systems.
文摘Even though a lot of research has been carried out concerning the preparation of carbonate apatite (CHA), they were related to CHA in the form of powder. In the present study, macroporous CHA bone substitutes were prepared through composition-transformation of gypsum and Ca-hydroxide. Here, we investigated the effect of added Ca-hydroxide to gypsum, carbonation periods, and hydrothermal temperatures for phosphatization to understand the basic principle of composition-transformation of gypsum added Ca-hydroxide to fabricate CHA bone substitutes. The specimens were characterized in terms of chemical and physical properties, such as extent of transformation of macroporous gypsum added Ca-hydroxide into CHA body, type and content of carbonate, and crystal morphology. It was observed that the transformation was faster with higher hydrothermal temperature. However, higher hydrothermal temperature caused de-carbonation phenomena which resulted in the lack of carbonate ions of the product. Moreover, the higher the percentage of Ca-hydroxide added to gypsum, caused the complete transformation of gypsum into CHA to be slower. These findings have been applied to the standard fabrication procedure of carbonate apatite, which in turn will allow scaling up process, and will be provided for biomedical purposes for the Indonesian community.
文摘The precursor of ammonium aluminum carbonate hydroxide was synthesized by using aluminum sulfate（Al2（SO4）3） and ammonium carbonate（（NH4）2CO3）. The effects of α-Al2O3 seeds and mixture composed of α-Al2O3 and ammonium nitrate, as well as multiplex catalysts （AT） on phase transformation of alumina in sintering process were investigated respectively. The results show that the α-Al2O3 seeds and the mixture of α-Al2O3 and ammonium nitrate can lower the phase transformation temperature of α-Al2O3 to different extents while the particles obtained agglomerate heavily. AT has great potential synergistic effects on the phase transformation of alumina and reduces the phase transformation temperature of α-Al2O3 and the trends of necking-formation between particles. Therefore the dispersion of powder particles is improved significantly.
文摘Energy density and production cost for high-performance electrode materials are the main challenge for the capacitive storage technology. In this paper, novel Hydroxide Zinc Carbonate (Zn4CO3(OH)6·H2O, HZC) catalyst layers, which are composed of irregular stagger arrangement nanosheets, have been synthesized successfully on foam Ni from inorganic precursors by a feasible in situ hydrothermal method. Measured by electrochemical tests as electrode materials for supercapacitors, the HZC@Ni foam show high specific capacitance (1329.2 F·g−1 at 1 A·g−1 and 882.8 F·g−1 at 10 A·g−1, respectively). These results show that the HZC@Ni foam could be a potential electrode material for supercapacitors. These encouraging results make these low-cost and eco-friendly materials promising for energy storage application.
基金Funded by the National Natural Science Foundation of China(No.51604087)the Science and Technology Program of Guangdong Province of China(No.2016A010104019)the Science and Technology Program of Guangzhou City of China(No.201607010001)
文摘Alpha nickel hydroxide has better performances than commercial beta nickel hydroxide. However, the main defect is that α-phase is difficult to synthesize and easily transformed to β-phase Ni（OH）2 upon aging in a strong alkaline solution. In this study, the Al-Co, Al-Yb, Yb-Co and Al-Yb-Co multiple doping was used respectively. By controlling the amount of sodium carbonate, the α-Ni（OH）2 was prepared by ultrasonic-assisted precipitation. And the influence of sodium carbonate on the crystalline phase and structure stability for alpha nickel hydroxide was studied. The results demonstrate that, with increasing amount, the biphase nickel hydroxide transforms to pure alpha nickel hydroxide gradually, and the structure stability is also improved. When the amount of sodium carbonate is 2 g, the sample still keeps α-Ni（OH）2 after being aged for 30 days, for Al-Yb-Co-Ni（OH）2. And when the amount is less than 2 g, the phase transformations exist in the samples with different extents. These results demonstrated that the amount of sodium carbonate is a critical factor to maintain the structural stability of α-Ni（OH）2.
基金supported by National Key R&D Program of China(2021YFA1502803)the National Natural Science Foundation of China(NSFC)(21972066 and 91745202)+3 种基金NSFC-Royal Society Joint Program(21661130149)Luming Peng thanks the Royal Society and Newton Fund for a Royal Society-Newton Advanced Fellowshipsupported by the Research Funds for the Frontiers Science Center for Critical Earth Material Cycling,Nanjing Universitya Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Layered double hydroxides(LDHs)have received extensive attention in many fields such as catalysis,environmental management and medical applications.Typically,expensive soluble metal salts are commonly used as the starting materials for the synthesis of LDHs.Here,we report a novel synthesis route for Mg/Al-LDH by using inexpensive basic magnesium carbonate as the starting material.X-ray diffraction(XRD)and solid-state nuclear magnetic resonance(ssNMR)data show that LDHs with rich defects are formed rapidly at room temperature and good crystallinity can be obtained after further hydrothermal treatment.These results provide a simple,rapid and green preparation method for LDHs.
文摘A novel type of composite electrode based on nmltiwalled carbon nanotubes coated with sheet-like cobalt hydroxide particles was used in supercapacitors. Cobalt hydroxide cathodlcally deposited fiom Co（NO3）O2 solution with carbon nanotubes as matrix exhibited large pseudo-capacitance of 322 F/g in 1 mol/L KOH. To characterize the cobalt hydroxide nanocomposite electrode, a charge-discharge cycling test, cyclic voltammetry, and an impedance test were done. This cobalt hydroxide composite exhibiting excellent pseudo-capacitive behavior （i.c. high reversibility, high specific capacitance, low impedance）, was demonstrated to be a candidate for the application of electrochemical supercapacitors. A combined capacitor consisting of cobalt hydroxide composite as a cathode and activated carbon fiber as an anode was reported. The electrochemical pcrformance of the combined capacitor was characterized by cyclic voltammetry and a dc charge/discharge test. The combined capacitor showed ideal capacitor behavior with an extended operating voltage of 1.4 V. According to the extended operating voltage, the energy density of the combined capacitor at a current density of 100 mA/cm^2 was found to be 11 Wh/kg. The combined capacitor exhibited high-energy density and stable power characteristics,
基金Funded by the National Natural Science Foundation of China(No.NNSF-51272194)
文摘The increasing importance of the ecologically minded production of building materials makes it necessary to develop reasonable alternatives to the CO2-intense production of ordinary Portland cement （OPC）. The development of new or modified concrete is an important part of existing strategies to improve performance and minimize life-cycle costs. Therefore, we investigated carbonation resistance properties of sulphoaluminate cement （SAC） concrete incorporating layered double hydroxides （LDHs）. X-ray diffraction （XRD） and IR-spectroscopy were employed to characterize the component and structural changes of LDHs and cement paste before and after carbonation test. Carbonation resistance of concrete was experimentally evaluated. Finally, carbonation of Portland cement and SAC concrete was compared. The experimental results show that carbonation depth decreases remarkably with the addition of LDHs, especially the calcinated LDHs. Carbonation depth of SAC concrete is smaller than that of PC concrete regardless of curing time.
基金Project(21471162) supported by the National Natural Science Foundation of ChinaProject(2015H6016) supported by the Science and Technology Project of Fujian Province,China
文摘A new design route was presented to fabricate cobalt aluminum-layered double hydroxide(CoAl-LDH)thin layers whichgrow on carbon spheres(CSs)through a growth method.The CoAl-LDH thin layers consist of nanoflakes with a thickness of20nm.The galvanostatic charge-discharge test of the CoAl-LDH/CSs composite shows a great specific capacitance of1198F/g at1A/g(based on the mass of the CoAl-LDH/CSs composite)in6mol/L KOH solution,and the composite displays an impressive specificcapacitance of920F/g even at a high current density of10A/g.Moreover,the composite remains a specific capacitance of928F/gafter1000cycles at2A/g,and the specific capacitance retention is84%,indicating that the composite has high specific capacitance,excellent rate capability and good cycling stability in comparison to pristine CoAl-LDH.
基金Funded by the National Natural Science Foundation of China(51172096)the Ministry of Education Program for New Century Excellent Talentsthe Fundamental Research Funds for the Central Universities
文摘Mineral carbonation using waste cement is a promising method to solve the problems caused by CO_2 emission and waste cement. Compaction pressure is an important parameter for mineral carbonation of calcium hydroxide, one of the most dominant composite of waste cement that can be carbonated. The carbonation degree, morphology of products and compressive strength of carbonated compacts are influenced by compaction pressure significantly. Results show that the carbonation degree of calcium hydroxide increases at first（0-8 MPa） and then decreases in the higher compaction pressure range（10-14 MPa）. At the meantime, results also indicate that lower compaction pressure accelerates the early carbonation but hinder carbonation in the later stages. For the morphologies of carbonation products, calcium carbonate tends to form typical crystal morphology of calcite（rhombohedral） under lower compaction pressure, while it will become ellipsoidlike when compaction pressure reaches 8 MPa. TGA and water content results show that there is an optimal water content for the carbonation. In addition, lower water content is adverse to the carbonation at later stage and the CO_2 is difficult to penetrate into the inside of compacts when water content is high, which will hinder the carbonation. XRD and TGA results show that the carbonation products are calcite and small amount of amorphous calcium carbonate.
文摘The glassy carbon (GC) electrode modified with a monolayer nickel hydroxide (GC/Ni(OH) 2) was prepared by immersion of GC substrate in 1.0×10 -3 mol/L NiSO 4 solution, and then cyclic voltammetric scanning in 0.20 mol/L KOH. Similarly, GC/Co(OH) 2 electrode was prepared too. The experiments showed that the voltammetric behavior of GC/Ni(OH) 2 electrode in 0.20 mol/L KOH is more stable than that of GC/ Co(OH) 2. It was found that the GC/Ni(OH) 2 electrode acts as an effective electrocatalysis for the oxidation of hydrazine.
基金Project(20090450188)supported by China Postdoctoral Science FoundationProject supported by Postdoctoral Science Foundation of Central South University,ChinaProject(0991247)supported by Natural Science Foundation of Guangxi Province,China
文摘Nickel hydroxide doped with multi-wall carbon nanotubes(MCNTs)was synthesized by chemical coprecipitation method. The MCNTs doped nickel hydroxide was used as the electrochemical active material in the positive electrodes of rechargeable alkaline batteries.The powder X-ray diffraction(XRD)analysis shows that the addition of MCNTs induces more structural defect within the crystal lattice of the nickel hydroxide.The cyclic voltammetry(CV)and electrochemical impedance spectroscopy(EIS) tests demonstrate the better reaction reversibility and lower electrochemical impedance of MCNTs doped nickel hydroxide as compared with the pure nickel hydroxide.The charge/discharge tests show that MCNTs addition can improve the specific discharge capacity and increase the discharge voltage of the nickel hydroxide electrode.
文摘Ni/Mg/Al layered double hydroxides(LDHs) with different n(Ni)∶n(Mg)∶n(Al) ratio values were prepared via a coprecipitation reaction. Then Ni/Mg/Al mixed oxides were obtained by calcination of these LDHs precursors. Carbon nanotubes were produced in the catalytic decomposition of propane over the Ni/Mg/Al mixed oxide catalysts. The quality of as-made nanotubes was investigated by SEM and TEM. The nanotubes were multiwall with a high length-diameter ratio and appeared to be flexible. The catalytic activities of these mixed oxides increased with increasing the Ni content. The Ni/Mg/Al mixed oxide with the highest Ni content [n(Ni)/n(Mg)/n(Al)=1/1/1] showed the highest activity and the carbon nanotubes grown on its surface had the best quality.
