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1.
Ordered mesoporous silica-carbon (MSC) were used as supports of Ni based catalysts for dry reforming of methane (DRM) reaction. The effects of preparation method and precipitant on the catalysts are investigated. The physical and chemical properties are discussed based on the H2-TPR, FTIR, XRD, TEM, H2-TPD and N2 adsorption/desorption characterization. It is found that the preparation method and choice of precipitants affect the catalysts significantly in terms of the properties and catalytic performance in DRM reaction. In detail, the catalysts prepared by the precipitation method show more highly dispersed Ni particles and further better catalytic activity than the impregnated catalyst. That is attributed to the forming Ni3Si2O5(OH)4 nanoflakes in the catalyst precursors with the existence of alkaline precipitants. And this Ni3Si2O5(OH)4 species bind the support more tightly than NiO in the impregnated Ni/MSC catalyst. Moreover, the choice of precipitants also influences the form of Ni3Si2O5(OH)4 species in the catalysts. Specially, the strong electrolytic capacity of NaOH gives the most Ni3Si2O5(OH)4 nanoflakes formed in Ni-MSC-1 catalyst, which results in the most highly Ni dispersity and further highest catalytic activity. Besides, the strong interaction between the Ni3Si2O5(OH)4 species and support are also advantageous to the resist sintering and formation of carbon deposition, that is related to the good catalytic stability of catalysts.  相似文献   

2.
This work presents the effect of calcium and carbonate precursors on properties of CaCO3. The synthetic CaCO3 samples were transformed into CaO and tested their application to high-temperature CO2 capture. Four different sorbent precursors were investigated in this work, including calcium chloride (CaCl2) and calcium acetate (CaAc2) as calcium precursor, and sodium carbonate (Na2CO3) and urea (CO(NH2)2) as carbonate precursor. The results show that both calcium and carbonate precursors affect morphologies of CaCO3; CaCO3,Cl-Urea, and CaCO3,Cl-Na have calcite phase, whereas mixed-phases of calcite (30%) and vaterite (70%) are observed with CaCO3,Ac-Na, and aragonite is found with CaCO3,Ac-Urea. CaCO3,Cl-Na exhibits small cubic (rhombohedral) particle, CaCO3,Cl-Urea possesses spherical particle with rough surface, CaCO3,Ac-Na has spherical-like morphology with smooth surface, and CaCO3,Ac-Urea possesses aggregated form of CaCO3 particles. For application to CO2 capture, CaO derived from CaCO3,Ac-Urea provides the highest CaO conversion of 80% at 700 °C. The synthetic CaO-based sorbents were further incorporated with nickel oxide to form one-body bi-functional catalysts for H2 production from sorption-enhanced steam ethanol reforming. The results show that 87%H2 purity could be obtained with pre-breakthrough period of 60 min. Sorbent reactivity can be maintained the production of H2 for at least 10 consecutive cycle tests.  相似文献   

3.
Sorption enhanced water gas shift reaction (SEWGS) based on calcium looping is an emerging technology for hydrogen production and CO2 capture. SEWGS involves mainly two reactions, the catalytic WGS reaction and the bulk carbonation of CaO with CO2, and the solid product is CaCO3, and the Ca(OH)2 may be formed from the reaction of CaO with H2O with the presence of steam in gas phase. The effect of Ca(OH)2 and CaCO3 on the catalytic WGS reaction and carbonation reaction was studied in a fluidized bed reactor. It was found that the hydrated sorbent and CaCO3 did not show any catalytic reactivity toward WGS reaction at 400 °C. When the temperature was increased to 500 °C and 600 °C, the catalytic reactivity of hydrated sorbent was recovered partially, but this will depend on the steam fraction in gas phase, the recovery of fresh CaO surface from dehydration of Ca(OH)2 may be the reason of catalytic reactivity recovery. CaCO3 can catalyze the WGS reaction at the high-temperature (>600 °C), this may due to the CaCO3 decomposition and recarbonation processes in which the CaO is transiently formed. The possible mechanism was discussed.  相似文献   

4.
Palm empty fruit bunch (EFB), a by-product of the palm oil industry, is being recognized as one of the most potential kinds of biomass for energy production in Thailand. However, it has been reported that, in combusting EFB in boilers, some compounds evolving from abundant alkali metals in EFB into gas-phase condense and deposit on low-temperature surfaces of heat exchange equipment, causing fouling and corrosion problems. To come up with a solution to impede the deposition, kaolin, which is abundant in kaolinite (Al2Si2O5(OH)4), is employed to capture the alkali metal vapours eluding from the combustion region. The experiments were designed to simulate the combustion situations that may take place when kaolin is utilized in two different approaches: premixing of kaolin with EFB prior to combustion and gas-phase reaction of volatiles from EFB with kaolin. The amounts of kaolin used were 8% and 16% by weight based on dry weight of EFB, which were equivalent to one and two times of the theoretical kaolin requirement to capture all potassium originally present in the EFB. The furnace temperatures used for EFB combustion were 700–900 °C and ashes were analyzed by XRF and XRD. The results revealed that, under the kaolin premixing condition, 8% kaolin addition was sufficient to capture the potassium compounds at low temperature, i.e. 700 and 800 °C. However, when the temperature was increased to 900 °C, 16% kaolin addition was needed to completely capture the potassium compounds. The results from gas-phase experiments showed that kaolin can capture volatile potassium at maximum 25% at 900 °C. The XRD results showed, for both experimental cases, the evidence of formation of the high melting temperature potassium-alumino-silicates, which confirmed the reaction of potassium compounds with kaolin. The study also suggests that the premixing method is better than the other because of its higher overall capture efficiency.  相似文献   

5.
Hydrogen has attracted significant attention as a clean energy source. Supercritical water gasification (SCWG) technology can produce hydrogen-rich gas while also disposing of sludge. The hydrogen yield from the SCWG of sludge is greatly increased when catalyzed by AlCl3. In this paper, a combined catalyst based on AlCl3 was proposed to further increase the hydrogen yield of SCWG of dewatered sewage sludge (DSS). Analysis of the products from catalytic gasified of DSS and its model compounds were used to propose a catalytic mechanism and reaction pathway of the catalytic SCWG of DSS. Among the combined catalysts used for the SCWG of DSS, 10 wt% AlCl3–H2O2 (mass ratio 8:2) had the best hydrogen production effect, and the hydrogen yield reached 8.88 mol/kg organic matter. This was 14% higher than when catalyzed by 10 wt% AlCl3. During catalysis with AlCl3, Al3+ reacted with OH in water and precipitated as Al(OH)3, which produced an acidic environment in the liquid product. Al(OH)3 dehydrated to form an AlO(OH) and deposited in the solid product. A small amount of H2O2 promoted the steam reforming reaction of organic matter in DSS, which increased the hydrogen yield. H2O2 further promoted the hydrogen yield in an acidic environment. The catalytic effect of AlCl3 was unaffected by H2O2. The H+ generated by AlCl3 during catalysis promoted H2O2 to further depolymerized organic matter (such as humic substances) in DSS, so that AlCl3–H2O2 catalyzed the SCWG of DSS to further increase the hydrogen yield. The order of hydrogen yield catalyzed by AlCl3–H2O2 was guaiacol > humic acid > glycerol > alanine > glucose. Compared with AlCl3, AlCl3–H2O2 reduced the hydrogen yield of glucose by nearly 20% and increased the hydrogen yield of humic acid by about 17% (25.81 mol/kg feed).  相似文献   

6.
Electrolytes containing LiB(C2O4)2 (LiBOB) salts are of increasing interest for lithium-ion cells for several reasons that include their ability to form a stable solid electrolyte interphase on graphite electrodes. However, cells containing these electrolytes often show inconsistent performance because of impurities in the LiBOB salt. In this work we compare cycling and impedance data from cells containing electrolytes with LiBOB that was obtained commercially and LiBOB purified by a rigorous recrystallization procedure. We relate the difference in performance to a lithium oxalate impurity that may be a residual from the salt manufacturing process. We also examine the reaction of LiBOB with water to determine the effect of salt storage in high-humidity environments. Although LiBOB electrolytes containing trace amounts (∼100 ppm) of moisture appear relatively stable, higher moisture contents (∼1 wt%) lead to observable salt decomposition resulting in the generation of B(C2O4)(OH) and LiB(C2O4)(OH)2 compounds that do not dissolve in typical carbonate solutions and impair lithium-ion cell performance.  相似文献   

7.
The carbonate looping process is a promising technology for CO2 capture. The decay of sorbents reactivity over multiple cycles is an obstacle for realizing the carbonate looping process. In this work, the reactivity and stability of carbide slag for CO2 capture have been examined. The results show that carbide slag exhibits superior CO2 capture performance even at severe calcination temperatures in comparison with limestones, shells, pure CaCO3, and Ca(OH)2. X-ray diffraction analysis shows that there is mayenite (Ca12Al14O33) formed in the calcination step for carbide slag, which is the main reason for its high stability in the carbonate looping process.  相似文献   

8.
One-step hydrothermal reaction has successfully been used to prepared three-dimensional hierarchitecture Co2(OH)3Cl@FeCo2O4 composite without any annealing treatment. The samples are investigated to confirm the crystal structure, elemental composition, morphology structure and electrochemical performance. The results show the sample has a three-dimensional hierarchitecture that nanoblocks are assembled with nanoparticles. And the specific surface area is 87.5 m2 g−1 and the total pore volume is 0.17 cm3 g−1. Meanwhile, the composite shows a high specific capacitance of 1110.0 F·g−1 at 1 A·g−1 and great cycling stability with 98.8% capacitance retention after 3000 cycles. To evaluate the electrochemical performances, the results are used to compare with the Co2(OH)3Cl and FeCo2O4 nanomaterials, indicating a higher capacitance and longer cycle stability shown by the as-synthesized sample. The as-synthesized Co2(OH)3Cl@FeCo2O4 composite has an outstanding electrochemical performance, predicting an enormous potential and promising future as a novel electrode material applied in supercapacitor.  相似文献   

9.
Modified Ca-based sorbents were obtained by adding sodium alkali into Ca(OH)2 and CaCO3. Reactive properties of modified Ca-based sorbents with acidic gases were investigated through reacting with gaseous HC1 at 450-760℃, and SEM and XRD technologies were adopted to get information on the reaction mechanism. Experimental data showed that HC1 dry removal efficiencies increased with temperature before 700℃ for all of the investigated sorbents, and there existed improved sorbents that corresponded to the highest removal efficiencies under the similar conditions. SEM photographs exhibited morphology difference between original and improved sorbents both before and after the reaction; and displayed that improved sorbents formed more porous product layers than original sorbents especially at higher temperature when product sintering became heavier, which is favorable to HC1 dry removal. XRD analysis showed that (1) improved Ca(OH)2 and CaCO3 were less crystalline than original lime and limestone; (2) the re  相似文献   

10.
In order to investigate effects of morphology and crystalline phase of different Ni-phyllosilicate catalysts on the catalytic performance for CO2 methanation, nanotubular Ni-phyllosilicate and MCM-41 supported Ni-phyllosilicate were synthesized through hydrothermal reaction of sodium silicate or MCM-41 with nickel nitrate. On one hand, nanosheets attributing to 2:1 type nickel phyllosilicate (Ni3Si4O10(OH)2·5H2O) were uniformly grown on the surface of MCM-41 spheres to form the MCM-41 supported Ni-phyllosilicate (Ni/M). On the other hand, 1:1 type Ni-phyllosilicate with nanotubular morphology (Ni/N) was synthesized through the reaction of Na2SiO3 and nickel nitrate. After a series of tests and characterizations, it was found that Ni/N exhibited low thermal stability and poor anti-sintering property, leading to poor catalytic activity for CO2 methanation. On the contrary, Ni/M was very stable, which obtained unchanged morphology and fine Ni particles after 750oC-reduction, resulting in high catalytic activity and long-term stability for CO2 methanation. In all, morphology and crystalline phase of Ni-phyllosilicate obviously affected catalytic performance, and the supported Ni-phyllosilicate catalyst was much better than the nanotubular Ni-phyllosilicate for CO2 methanation in this work.  相似文献   

11.
Hydrothermal synthesis of CuV2O6 supported on 3-D ordered mesoporous SiO2 (CuV/SiO2) was studied to evaluate the catalytic activity for SO3 decomposition, which is a key step in solar thermochemical hydrogen production. A composite oxide hydrate, Cu3O(V2O7)·H2O, and an oxide hydroxide hydrate, Cu3(OH)2V2O7·(H2O)2, were formed at lower hydrothermal temperatures (≤200 °C). The oxide hydrate phase mainly yielded Cu2V2O7 after calcination at 600 °C in air. By contrast, the hydrothermal synthesis at 250 °C (CuV/SiO2@250) directly crystallized CuV2O6 from the oxide hydroxide hydrate, although its very large particle size (∼5 μm) is not suitable for the catalytic application. The SO3 decomposition activity measured at 600 °C was associated with the yield as well as the dispersion of CuV2O6, giving rise to the maximum for the hydrothermal synthesis at 200 °C. CuV/SiO2@250 achieved the highest catalytic activity at the reaction temperature of 650 °C, because the melting phase of CuV2O6 penetrated mesoporous SiO2 and thus improved the dispersion of the active phase.  相似文献   

12.
In order to better understand the pathways of hydrothermal gasification of cellulose, the effect of headspace fraction and alkalinity on the hydrothermal gasification of cellulose has been studied at 315 °C in the presence of Pt/Al2O3 as catalyst. It was found that regardless of alkalinity the headspace fraction had a large impact on gasification yield, with larger headspace fractions resulting in considerably more gas product. Without the addition of sodium carbonate, the effect of headspace fraction became more pronounced, with gas increasing by approximately a factor of forty from the lowest to highest headspace fraction. On the other hand, for the same residence time the addition of sodium carbonate co-catalyst dampened the magnitude of the effect, to a factor of 2.5 and 1.5, for 50 and 100 mM sodium carbonate solutions, respectively. These results indicated that the headspace fraction affected the phase behaviour, and that this altered the pathway of the cellulose decomposition. While furfural alcohol was the major product obtained with a 49% headspace fraction, it was effectively suppressed by using 78% or greater headspace fractions. Based on the effects of phase behaviour and previous literature, the reduced effect occurring upon the addition of sodium carbonate may relate to catalysis of the Lobry de-bruyn Van Eckenstein transform to produce lactic acid rather than intermediates proceeding through glycolaldehyde.  相似文献   

13.
Strategies of H2 production and CO2 mineralization were combined through olivine [(Mg,Fe)2SiO4] serpentinization and carbonation in a CO2-rich hydrothermal system. However, natural mantle peridotites commonly contain not only olivine but also orthopyroxene and/or clinopyroxene, which have effects that are not well understood. The present study investigated the reactions in H2O-olivine/orthopyroxene-CO2 systems by performing hydrothermal experiments in 0.5 M NaHCO3 solutions at 300 °C and 10 MPa.The yields of H2 and HCOOH initially were first suppressed in the presence of orthopyroxene; however, after orthopyroxene consumption, the rate of H2 production increased significantly. H2 yield increased to 348.3 mmol/kgmineral in 120 h with the presence of 20 wt% orthopyroxene at the beginning of the reaction. The initial suppression of H2 generation was due to incorporation of more Fe(II) into serpentine [(Mg,Fe)3Si2O5(OH)4] in the high SiO2(aq) concentration system. The presence of orthopyroxene also dramatically accelerated serpentine formation. In contrast, magnesite [(Mg,Fe)CO3] formation was inhibited upon addition of orthopyroxene, which also contributed to the release of Fe(II). Therefore, peridotite containing ≤20 wt% of pyroxenes is more suitable for long-term H2 production than pure olivine. When considering the reaction output of a water-peridotite-CO2 system, controlling the percentage of pyroxenes in the starting mineral may be more important than expected.  相似文献   

14.
A new photoelectrochemical system based on semiconductor photocathodes (p-Si, p-InP) and an electron carrier (mediator) is proposed. Aqueous solutions of heteropolyacids (HPA): H4(PMo12O42), H8(SiW12O42), H7(PW12O42) and H8(SiMo12O42) were examined for use as mediators. The electrons generated in the semiconductor upon illumination reduce HPA. This reaction proceeds at a lower overvoltage than the direct hydrogen photoevolution from aqueous acid solution. The mediator reduction on the photocathode is followed by a homogeneous dark chemical reaction between the reduced mediator and water, which results in hydrogen evolution. The catalytic activity of the photocathodes investigated towards electroreduction of HPA increases after deposition of platinum traces on the working surface of the electrode.  相似文献   

15.
《能源学会志》2020,93(6):2536-2543
Coal blending is an effective method to reduce the slagging tendency. The mineral transformation within blended coal ashes has an important influence on the slagging behaviors, which have been well studied under conventional air-fuel condition. Oxy-fuel combustion is recognized as one of the most promising CO2 reduction technologies. However, the mineral transformation within blended coal ashes in oxy-fuel condition has yet to be fully understood. This work is aimed to comprehensively study the influence of CO2 atmosphere on Ca-containing mineral transformation behaviors during a Ca dominated coal co-firing with a Si/Al dominated coal in O2/CO2 condition by TG-DSC, XRD and HSC simulation. These results show that the atmosphere significantly affects on the transformation of Ca-containing mineral and the final existing form of Ca in the blended coal ashes. When the high content Ca coal is blended with the high content Al/Si coal in the O2/CO2 atmosphere, the CO2 promotes the transformation of Ca into CaCO3 and Ca under low temperature mainly exists in the form of CaCO3 (little CaSO4) in the blended coal ashes. CaCO3 under high temperature is decomposed to produce highly active CaO, and CaO reacts with Al/Si to form the low melting point minerals, which may aggravate the slagging tendency. The present study can provide useful information to reduce the slagging behavior of the blended coals in the O2/CO2 atmosphere.  相似文献   

16.
Photocatalytic hydrogen production was investigated over ZnS1−x−0.5yOx(OH)y-ZnO using sulfide ion (Na2S-Na2SO3) as an electron donor from NaCl saltwater. NaCl can affect markedly the activity for photocatalytic hydrogen production, depending on NaCl concentration. When NaCl concentration is lower, the activity is lower than that in pure water, whereas when NaCl concentration is higher, the activity is higher than that in pure water. NaCl decreases not only the surface charge of ZnS1−x−0.5yOx(OH)y-ZnO but also the surface hydration. When ZnS1−x−0.5yOx(OH)y-ZnO was impregnated with the electron donor (Na2S-Na2SO3), ZnO was transformed partly into ZnS. The impregnated ZnS1−x−0.5yOx(OH)y-ZnO exhibits higher activity than the non-impregnated one. The possible mechanisms were discussed.  相似文献   

17.
Design and direct construction of oxygen evolution reaction (OER) catalyst-based electrode is an efficient route to improve the water splitting reaction. Herein, we proposed a facile route to synthesize and load the composite of amorphous CoFe oxyhydroxide (CoFeOx(OH)y) and MoS2 on the carbon paper by combining a hydrothermal and an electrodeposition process. CoFeOx(OH)y has a special feature of long-range disorder (amorphous phase) and short-range order (crystal phase), which greatly improves the OER catalytic performance of the hybrids. In virtue of the synergistic effect of CoFeOx(OH)y and MoS2, an improved electronic coupling effect occurs, which increases the oxidation state of Co and Fe, and thus enhances OER activity. As-synthesized CoFeOx(OH)y/MoS2/CP (CFOMS/CP) electrode affords excellent electrocatalytic activity and good electrochemical OER stability: A small Tafel slope of 37.9 mV dec?1 (vs. 62.1 mV dec?1 for CoFeOx(OH)y/CP, 120.2 mV dec?1 for RuO2/CP) and low overpotential 242 mV at 10 mA cm?2 (vs. 263 mV for CoFeOx(OH)y/CP, 317 mV for RuO2/CP), as well as a stable running for 25 h.  相似文献   

18.
a low-cost electrode with lawn-like NiS2 nanowire arrays on flexible carbon fiber paper was synthesized, for the first time, via sulfurization of Ni2(CO3)(OH)2 precursor. And the performance of this electrode as a bifunctional electrocatalyst toward both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) was evaluated. It shows that NiS2 NWs/CFP requires small overpotentials of 165 mV for HER and 246 mV for OER, respectively, to deliver the current density of 10 mA cm?2 in 1.0 M KOH. The corresponding symmetric two-electrode alkaline water electrolyzer only needs a cell voltage of 1.59 V to afford 10 mA cm?2 water-splitting current density.  相似文献   

19.
Nano particles of Ru, Rh, Pd, Ir, Pt, and Au, protected by polyvinyl pyrrolidone (PVP), were applied to the hydrodeoxygenation of cellulose and xylan in water and 5 MPa H2 at 543 K. The distributions of products generated from cellulose and xylan were roughly similar to each other under the present reaction conditions, and therefore, the former was intensively studied. The Ru-PVP catalyst afforded mainly methane and lower alkanes, rather than producing water soluble organic compounds, such as diols and alcohols, that were formed with the use of the other catalysts. The changes in the product distributions with reaction temperature and time indicated that the reaction consisted of two consecutive reactions: cellulose or xylan → water soluble compounds → hydrogenolysis. The first transformation was promoted in subcritical water, and the second step was catalyzed by the Ru catalyst. The Ru catalyst that was supported on CeO2, γ-Al2O3, or activated carbon yielded a similar product distribution to that on Ru-PVP; however, the loading of Ru on TiO2, ZrO2, SiO2–Al2O3, or SiO2 resulted in the increment of diols. After the reaction a small portion of the CeO2 and most of the SiO2–Al2O3 and SiO2 were dissolved in water, and a portion of the Al2O3 was transformed to boehmite AlO(OH) from the γ-alumina. Little change in the catalytic activity however was observed upon the reuse of Ru/Al2O3 in the second run.  相似文献   

20.
The main factors limiting water splitting producing hydrogen production are overpotential, activity and persistence of electrocatalysts. Herein, a novel NixCo1-x(OH)2 coupled with NiFe amorphous compound array growing on nickel foam substrate (expressed as NixCo1-x(OH)2/NiFe-AM) was developed by facile hydrothermal and electrodeposition methods. Significantly, NixCo1-x(OH)2/NiFe-AM with this unique structural exhibits superior activity and stability in the two half reactions of water electrolysis. In addition, when tested in an alkaline electrolyte with a current density of 10 mA cm−2, the overpotentials of HER and OER was 157 mV and 196 mV (60 mA cm−2), respectively. The stability can up to 60 h. These test results show through constructing hierarchical nano-thron architecture enhanced electrocatalytic activity to produce hydrogen and oxygen.  相似文献   

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