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1.
This study aimed to evaluate the effect of the organic loading rate (OLR) (60, 90, and 120 g Chemical Oxygen Demand (COD). L?1. d?1) on hydrogen production from cheese whey and glycerol fermentation as cosubstrates (50% cheese whey and 50% glycerol on a COD basis) in a thermophilic fluidized bed reactor (55 °C). The increase in the OLR to 90 gCOD.L?1. d?1 favored the hydrogen production rate (HPR) (3.9 L H2. L?1. d?1) and hydrogen yield (HY) (1.7 mmol H2. gCOD?1app) concomitant with the production of butyric and acetic acids. Employing 16S rRNA gene sequencing, the highest hydrogen production was related to the detection of Thermoanaerobacterium (34.9%), Pseudomonas (14.5%), and Clostridium (4.7%). Conversely, at 120 gCOD.L?1. d?1, HPR and HY decreased to 2.5 L H2. L?1. d?1 and 0.8 mmol H2. gCOD?1app, respectively, due to lactic acid production that was related to the genera Thermoanaerobacterium (50.91%) and Tumebacillus (23.56%). Cofermentation favored hydrogen production at higher OLRs than cheese whey single fermentation.  相似文献   

2.
The use of multi-pore nanostructured g-C3N4 photocatalysts is an efficient approach to separate photogenerated charge carriers and increase visible light photocatalytic performance. Recent progress has yielded nanostructured material through hard templating, which limits potential applications. Integrating the 2D building block into multidimensional porous structures remains a significant challenge in scalable production. Herein, a novel technique based on P407 bubble clusters templating and fixation by freezing is described for the first time to fabricate a 3D opened-up macroporous g-C3N4 nanostructures for photocatalytic H2 evolution. Three-dimensional hierarchical nanostructures provide more contact active sites and synergistically promote the creation of heterogeneous catalytic interfaces. This feature is very useful for understanding the transfer path of photoinduced charges as well as the origins of the high charge separation efficiency in photocatalytic reactions, thus yielding a remarkable visible light-induced H2 evolution rate of 4213.6 μmol h−1 g−1, which is nearly 5.6 times (716 μmol h−1 g−1) higher than that of lamellar bulk g-C3N4. This newly developed approach offers a promising alternative to synthesize broad-spectral response 3D hierarchal g-C3N4 nanostructures and can be extended to assemble other functional nanomaterials as building blocks into macroscopic configurations coupled with electronic modulation strategy simultaneously.  相似文献   

3.
TiO2 quantum dots-sensitized Cu2S (Cu2S/TiO2) nanocomposites with varying concentration of TiO2 QDs are synthesized via a facile two-stage hydrothermal-wet impregnation method. X-ray diffraction analysis confirms the formation of Cu2S and TiO2with chalcocite and anatase phases, respectively. The observed shoulder-like absorption peaks indicate the UV–visible light-driven properties of the composite. Morphological analysis reveals that the fabricated Cu2S/TiO2 composite consists of Cu2S with a nano rod-like shape (average length and width of ~856 and ~213 nm, respectively) and nanosheets-like structures (average length and width of ~283 and ~289 nm, respectively), whereas the TiO2 is formed as quantum dots with a size range of 8.2 ± 0.4 nm. Chemical state analysis shows the presence of Cu+, S2?, Ni2+, and O2? in the nanocomposite. The H2 evolution rate over the optimized photocatalyst is found to be ~45.6 mmol h?1g?1cat under simulated solar irradiation, which is around 5 and 2.4-fold higher than that of the pristine TiO2 and Cu2S, respectively. Continuous H2 production for 30 h is achieved during time-on-stream experiments, demonstrating the excellent stability and durability of the Cu2S/TiO2 photocatalyst for large-scale applications.  相似文献   

4.
The biological production of hydrogen by microalgae is considered as an advantageous process. However, its yields are sometimes limited. To go beyond this limit, the improvement of the H2 generation rate by Spirulina was studied via an electrochemical photo-bioreactor (EPBR). This EPBR led to hydrogen evolution rates of up to 27.49 and 13.37 mol of H2.d−1.m−3 for the anode and cathode chambers, respectively, under 0.3 V voltage and ~2.5 mA current. These results represent about a 4-fold increase compared to the H2 production rate recorded without the application of a voltage. This increase in bio-hydrogen production is correlated with a drop in the concentration of NADPH. The Electrochemical Sequential Batch Reactor (ESRB) provided a more interesting total production rate which was 2.65 m3 m−3 d−1, compared to the batch mode, which gave 1.2 m3 m−3.d−1. The results show, for the first time, the boosting effect of the voltage on the metabolism of H2 production by the Spirulina strain.  相似文献   

5.
Conjugated polymers have emerged as a promising class of organic photocatalysts for photocatalytic hydrogen evolution from water splitting due to their adjustable chemical structures and electronic properties. However, developing highly efficient organic polymer photocatalysts with high photocatalytic activity for hydrogen evolution remains a significant challenge. Herein, we present an efficient approach to enhance the photocatalytic performance of linear conjugated polymers by modifying the surface chemistry via introducing a hydrophilic adenine group into the side chain. The adenine unit with five nitrogen atoms could enhance the interaction between the surface of polymer photocatalyst and water molecules through the formation of hydrogen bonding, which improves the hydrophilicity and dispersity of the resulting polymer photocatalyst in the photocatalytic reaction solution. In addition, the strong electron-donating ability of adenine group with plentiful nitrogen atoms could promote the separation of light-induced electrons and holes. As a result, the adenine-functionalized conjugated polymer PF6A-DBTO2 shows a high photocatalytic activity with a hydrogen evolution rate (HER) of 25.21 mmol g?1 h?1 under UV-Vis light irradiation, which is much higher than that of its counterpart polymer PF6-DBTO2 without the adenine group (6.53 mmol g?1 h?1). More importantly, PF6A-DBTO2 without addition of a Pt co-catalyst also exhibits an impressive HER of 21.93 mmol g?1 h?1 under visible light (λ > 420 nm). This work highlights that it is an efficient strategy to improve the photocatalytic activity of conjugated polymer photocatalysts by the modification of surface chemistry.  相似文献   

6.
In recent times, biohydrogen production from microalgal feedstock has garnered considerable research interests to sustainably replace the fossil fuels. The present work adapted an integrated approach of utilizing deoiled Scenedesmus obliquus biomass as feedstock for biohydrogen production and valorization of dark fermentation (DF) effluent via biomethanation. The microalgae was cultivated under different CO2 concentration. CO2-air sparging of 5% v/v supported maximum microalgal growth and carbohydrate production with CO2 fixation ability of 727.7 mg L?1 d?1. Thereafter, lipid present in microalgae was extracted for biodiesel production and the deoiled microalgal biomass (DMB) was subjected to different pretreatment techniques to maximize the carbohydrate recovery and biohydrogen yield. Steam heating (121 °C) in coherence with H2SO4 (0.5 N) documented highest carbohydrate recovery of 87.5%. DF of acid-thermal pretreated DMB resulted in maximum H2 yield of 97.6 mL g?1 VS which was almost 10 times higher as compared to untreated DMB (9.8 mL g?1 VS). Subsequent utilization of DF effluent in biomethanation process resulted in cumulative methane production of 1060 mL L?1. The total substrate energy recovered from integrated biofuel production system was 30%. The present study envisages a microalgal biorefinery to produce biohydrogen via DF coupled with concomitant CO2 sequestration.  相似文献   

7.
Silicon-based nanosheets (SNS) were synthesised via a mild (60 °C) and time-saving (8 h) modified topochemical method. Then, Cu3(BTC)2 and SNS@Cu3(BTC)2 were successfully synthesised by microwave irradiation, and their characteristics and hydrogen storage performance were analysed by multiple techniques. The accordion-like SNS exhibited void spaces, a unique low buckled structure, and ultrathin, almost transparent, loosely stacked layers with a high specific surface area (362 m2/g). After in-situ synthesis with Cu3(BTC)2, the SNS compound achieved a high specific surface area (1526 m2/g), outstanding hydrogen storage performance (5.6 wt%), and a desirable hydrogen diffusion coefficient (10?7). Thus, SNS doping improved the hydrogen storage performance of Cu3(BTC)2 by 64% through electron transfer reactions with Cu enabled by the unique composite nanostructure of SNS@Cu3(BTC)2. This study presents a promising method of synthesising SNS and porous composite materials for hydrogen storage.  相似文献   

8.
Although utilization of diverse classes of metal oxides as hydrogen storage materials has been reported, but there is still a major need to introduce efficient materials. Herein, mesoporous Zn2V2O7 nanostructures were produced by a new sonochemical method using hydrazine, zinc nitrate, and ammonium vanadate as the starting reagents and then annealed at 700 °C. Prior to annealing, Zn3V3O8 was produced in the presence of ultrasonic waves, whereas in the absence of ultrasonic waves, Zn2(VO4)2 was the major product. In fact, ultrasonic waves interfered with the reaction mechanism and reduced V5+ to V4+ and V3+. Because of the proper composition and structure of these nanostructures, they were used for electrochemical storage of hydrogen. Storage of over 2899 mAh/g after 20 cycles by flower-like nanostructures revealed their high capability. The results also showed that morphology affects efficiency such that three-dimensional spherical nanostructures had a storage capacity of 2247 mAh/g after 20 cycles.  相似文献   

9.
To overcome the global challenges of energy crises and environmental threats, urea oxidation is a hopeful route to utilize urea-rich wastewater as an energy source for hydrogen production. Herein, we report an inorganic/organic type of nano-heterostructure (NHs–Ni-TiO2/p-NDIHBT) as a photoanode with excellent urea oxidation efficiency driven by visible light. This heterostructured photoanode consists of nickel (Ni)-doped TiO2 nanorods (NRs) arrays as an inorganic part and a D-A-D type organic polymer i.e p-NDIHBT as an organic part. The as-prepared photoanode was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The morphological studies of TEM confirm the coating of p-NDIHBT on Ni–TiO2 NPs (~1 μm). The consequence of heterostructure formation on optical and photoelectrochemical (PEC) properties of photoanode were explored through photoelectrochemical responses under visible light irradiation. The photoelectrochemical activity of Ni–TiO2 and Ni–TiO2/p-NDIHBT photoanode from linear sweep voltammetry (LSV) shows the ultrahigh photocurrent density of 0.36 mA/cm2 and 2.21 mA/cm2, respectively measured at 1.965 VRHE. Electrochemical impedance spectroscopy (EIS) of both photoanodes shows a highly sensitive nature toward the urea oxidation reaction. The hybrid photoanode also exhibits high photostability, good solar-to-hydrogen conversion efficiency, and high faradaic efficiency for urea oxidation.  相似文献   

10.
Here, we report the synergistic effect of dual TiO2 layers to enhance the PEC performance of Zirconium-doped zinc ferrite (ZZFO) photoanode by improving the charge carrier density and suppressing the photogenerated charge recombination. The TiO2 underlayer works as a blocking layer to remarkably suppress the back-injection of electrons from the fluorine-doped tin oxide (FTO) leading to reducing the bulk charge recombination. While interlayer TiO2 improves the bulk charge transfer property of ZZFO photoanodes. The optimal TiO2 double-layer modified ZZFO photoanode exhibits an enhanced photocurrent of 0.435 mA/cm2 at 1.23 V vs. reversible hydrogen electrode (RHE), which is 2.5 times higher than that of the ZZFO photoanode. The effect of each layer was deeply investigated by electrochemical impedance spectroscopy (EIS), intensity-modulated photocurrent spectroscopy (IMPS) and time-resolved photoluminescence studies (TRPL) with the aim of gaining a clear picture of the interface modifications and their impact on the efficiency of the ZZFO photoanode.  相似文献   

11.
Photocatalysts can be used both for air cleaning and solar energy harvesting through water splitting. However, pure TiO2 photocatalysts are often inefficient and therefore co-catalysts are needed to improve the yield. To achieve this goal, we prepared TiO2 and deposited Pt, Ir and Ru co-catalysts on its surface. Two base TiO2 nanoparticles were used: P25 and rutile TiO2 synthesized via hydrothermal method. Co-catalysts were deposited by wet impregnation technique using single element and a combination of two elements (Pt and Ir or Pt and Ru), followed by annealing in either air or H2/Ar. Annealing in reducing atmosphere increased the photocatalytic activity of oxidation of isopropanol compared to annealing in air. We demonstrated a clear influence of the co-catalysts on the photocatalytic degradation of isopropanol and on electrochemical water-splitting reaction. The platinum-containing samples showed the best HER activity.  相似文献   

12.
In recent years, a lot of scientific effort has been put into reusing the energy potential of sugarcane vinasse by dark fermentation. However, the findings so far indicate that new pathways need to be followed. In this context, this study assessed the effect of hydraulic retention time (HRT, from 24 to 1 h) on vinasse fermentation (10, 20, and 30 g COD L?1) in three mesophilic expanded granular sludge bed reactors (EGSB). The carbohydrate conversion remained above 60% at all organic loading rates applied. The maximum hydrogen production rate (8.77 L day?1 L?1) was obtained for 720 kg COD m?3 day?1 and associated to the lactate-acetate pathway. The highest productivities of propionic, acetic, and butyric acids were 3.11, 1.68, and 2.45 g L?1 h?1, respectively, at a HRT of 1 h. At this HRT, the degrees of acidification remained between 54% and 76% in all EGSB reactors. This research provides insights for carboxylate production from sugarcane vinasse and suggests applying the EGSB setup in the acidogenic stage of two-stage processes.  相似文献   

13.
ZIF-67 derived catalysts for Fischer-Tropsch synthesis have attracted much attention in recent years, while there is still a potential to improve their activity and selectivity. In this work, we prepared Si/Al co-immobilized Co3O4@SixAly catalysts by in-situ doping tetraethylorthosilicate and aluminum nitrate during the synthesis of ZIF-67. The effects of different Si/Al ratios on the metal-support interaction, acidity and FTS performance were explored. Results indicated that the Co3O4@Si0Al4 catalyst exhibited the best FTS performance with the CO conversion as high as 79.9% and CTY (cobalt time yield) value of 19.5 × 10?5 molCO·gCo?1·s?1, which was ascribed to the moderate metal-support interaction and the most active Co sites. Meanwhile, the Co3O4@Si3Al1 and Co3O4@Si2Al2 catalysts exhibited higher iso-paraffin and olefin selectivity due to more acidic sites.  相似文献   

14.
The objective of this study was to evaluate the effects of hydraulic retention time (HRT) (8–1 h) on H2 production from sugarcane juice (5000 mg COD L−1) in mesophilic (30 °C, AFBR-30) and thermophilic (55 °C, AFBR-55) anaerobic fluidized bed reactors (AFBRs). At HRTs of 8 and 1 h in AFBR-30, the H2 production rates were 60 and 116 mL H2 h−1 L−1, the hydrogen yields were 0.60 and 0.10 mol H2 mol−1 hexose, and the highest bacterial diversities were 2.47 and 2.34, respectively. In AFBR-55, the decrease in the HRT from 8 to 1 h increased the hydrogen production rate to 501 mL H2 h−1 L−1 at the HRT of 1 h. The maximum hydrogen yield of 1.52 mol H2 mol−1 hexose was observed at the HRT of 2 h and was associated with the lowest bacterial diversity (0.92) and highest bacterial dominance (0.52).  相似文献   

15.
The inefficient extracellular electron transfer (EET) is detrimental to power generation and waste degradation in microbial fuel cells (MFCs). Herein, we report a self-supporting anode for MFCs prepared by graphitization of steamed bread slices followed by in-situ polymerization to fabricate polyaniline@N-doped macroporous carbon foam (PANI@NMCF). The natural nitrogen-containing wheat flour was fermented and carbonized to form NMCF with a high specific surface area of 818.1 m2 g?1. After the NMCF surface modified by PANI, the enhanced hydrophilicity and conductivity of the PANI@NMCF anode would facilitate microbial adhesion, biofilm formation, and electron transfer. The surface improvements enhance the EET process for high-performance MFCs, including a short startup time of 21.7 h, high maximum output power density of 1160 ± 17 mW m?2, and decolourisation efficiency of 88.6 ± 1.2% for 36 h. The chemical oxygen demand removal efficiency was about 84.6 ± 1.1% at end of the operating cycles. This work provides a good foundation for our future development of carbon-based electrode materials for energy conversion and storage devices.  相似文献   

16.
《能源学会志》2020,93(6):2488-2496
The thermocatalytic alteration of CH4 into highly pure hydrogen and filaments of carbon was investigated on a series of Ni-catalysts with various contents (25, 40, 55, and 70 wt%) supported mesoporous spherical SiO2. The silica with ordered structure and high specific surface area (1136 m2/g) was synthesized using the Stöber technique with TEOS as a silica precursor and CTAB as the template in a simple synthesis system of aqueous-phase. This technique led to the preparation of mesoporous spherical silica. The prepared samples were characterized using BET, TPR, XRD, TPO, and SEM analyses. The prepared catalysts with different nickel loading showed the BET surface area ranging from 225.0 to 725.7 m2/g. These results indicated that an increase in nickel content decreases the surface area and leads to a subsequent collapse of a pore structure. SEM analysis confirmed a spherical nanostructure of catalysts and revealed that with the increase in loading of Ni, the particle size enlarged, because of the agglomeration of the particles. The results implied that the high methane conversion of 54% obtained over the 55 wt% Ni/SiO2 at 575 °C and this sample had higher stability at lower reaction temperature than the other prepared catalysts, slowly deactivation was observed for this catalyst at a period of 300 min of time on stream.  相似文献   

17.
Steam methane reforming (SMR) needs the reaction heat at a temperature above 800 °C provided by the combustion of natural gas and suffers from adverse environmental impact and the hydrogen separated from other chemicals needs extra energy penalty. In order to avoid the expensive cost and high power consumption caused by capturing CO2 after combustion in SMR, natural gas Chemical Looping Reforming (CLR) is proposed, where the chemical looping combustion of metal oxides replaced the direct combustion of NG to convert natural gas to hydrogen and carbon dioxide. Although CO2 can be separated with less energy penalty when combustion, CLR still require higher temperature heat for the hydrogen production and cause the poor sintering of oxygen carriers (OC). Here, we report a high-rate hydrogen production and low-energy penalty of strategy by natural gas chemical-looping process with both metallic oxide reduction and metal oxidation coupled with steam. Fe3O4 is employed as an oxygen carrier. Different from the common chemical looping reforming, the double side reactions of both the reduction and oxidization enable to provide the hydrogen in the range of 500–600 °C under the atmospheric pressure. Furthermore, the CO2 is absorbed and captured with reduction reaction simultaneously.Through the thermodynamic analysis and irreversibility analysis of hydrogen production by natural gas via chemical looping reforming at atmospheric pressure, we provide a possibility of hydrogen production from methane at moderate temperature. The reported results in this paper should be viewed as optimistic due to several idealized assumptions: Considering that the chemical looping reaction is carried out at the equilibrium temperature of 500 °C, and complete CO2 capture can be achieved. It is assumed that the unreacted methane and hydrogen are completely separated by physical adsorption. This paper may have the potential of saving the natural gas consumption required to produce 1 m3 H2 and reducing the cost of hydrogen production.  相似文献   

18.
The oxygen evolution reaction (OER) at anode requires high overpotential and is still challenging. The metallic core-oxyhydroxide layer structure is an efficient method to lower an overpotential. We synthesized Fe rich FeCo core-Co rich FeCo oxyhydroxide layer with a different particle size of 173 nm, 225 nm, and 387 nm (FeCo 173, 225, 387) through a difference in the reduction rate of Fe/Co precursors using facile modified polyol synthesis. To investigate the effect of conductivity, CoFe2O4 nanoparticles of 80–130 nm were synthesized. Among samples, FeCo 173 showed remarkable catalytic performance of 316 mV at a current density of 10 mA/cm2 in 0.1 M KOH compared to RuO2 (408 mV), FeCo 225 (323 mV), FeCo 387 (334 mV), CoFe2O4 (382 mV). Moreover, FeCo 173 showed good stability for 60,000 s while RuO2 showed a gradual increase in overpotential to maintain 10 mA/cm2 after 15,000 s in chronopotentiometry. The excellent performance was attributed to Fe-rich metallic core, a small amount of Fe doping into CoOOH, and the synergic effect between the active site of Co rich FeCoOOH and conductive Fe rich metallic core. Following this result, it shows that the use of such FeCo electrodes has advantages in the production of hydrogen via electrochemical water oxidation.  相似文献   

19.
Under certain conditions, cyanobacteria can switch from photosynthesis to hydrogen production, which is a good energy carrier. However, the biological diversity of hydrogen-releasing cyanobacteria has a great unexplored potential. This study is aimed to investigate the ability of new strains of cyanobacteria Cyanobacterium sp. IPPAS B-1200, Dolichospermum sp. IPPAS B-1213, and Sodalinema gerasimenkoae IPPAS B-353 to release H2 and to evaluate the effects of photosystem II inhibitor 3-(3,4-dichlorphenyl)-1,1-dimethylurea (DCMU) on H2 production under light and dark conditions. The results showed that cultures treated with DCMU produced several times more H2 than untreated cells. The highest rate of H2 photoproduction of 4.24 μmol H2 (mg Chl a h)?1 was found in a Dolichospermum sp. IPPAS B-1213 culture treated with 20 μM DCMU.  相似文献   

20.
In this study, highly active and stable CeO2, ZrO2, and Zr(1-x)Ce(x)O2-supported Co catalysts were prepared using the co-precipitation method for the high-temperature water gas shift reaction to produce hydrogen from waste-derived synthesis gas. The physicochemical properties of the catalysts were investigated by carrying out Brunauer-Emmet-Teller, X-ray diffraction, CO-chemisorption, Raman spectroscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and H2-temperature-programmed reduction measurements. With an increase in the ZrO2 content, the surface area and reducibility of the catalysts increased, while the interaction between Co and the support and the dispersion of Co deteriorated. The Co–Zr0.4Ce0·6O2 and Co–Zr0.6Ce0·4O2 catalysts showed higher oxygen storage capacity than that of the others because of the distortion of the CeO2 structure due to the substitution of Ce4+ by Zr4+. The Co–Zr0.6Ce0·4O2 catalyst with high reducibility and oxygen storage capacity exhibited the best catalytic performance and stability among all the catalysts investigated in this study.  相似文献   

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