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学者姓名:郭烈锦
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Abstract :
Supercritical water gasification (SCWG) was a promising technology to treat black liquor harmlessly and recycle energy efficiently, while the sulfur transformation of black liquor during SCWG process remained unknow. Herein, the effects of different parameters on gasification and sulfur transformation was determined in a batch reactor. The results showed that reaction temperature played the most important role. H-2 was the most important gaseous product with the maximum yields of 19.01 mol center dot kg(-1), simultaneously achieving the highest carbon gasification efficiency (95.16 %), COD removal rate (99.98 %) and the pH of 8.5 at 700 degrees C, 30 min and 25 MPa. After SCWG treatment, most of sulfur existed in the form of sulfide (H2S/S2-), and the maximum proportion of which was up to 90.51 % at 700 degrees C, 30 min and 25 MPa. With the increase in temperature, the organic sulfur (thiol/thioether, sulfone and thiophene) and inorganic sulfur (sulfate and thiosulfate) were transformed into sulfide (H2S/S2-). Finally, the sulfur transformation mechanisms of black liquor in SCWG were proposed. This work provided a basis for resource utilization of black liquor and a promising method for sodium sulfide production.
Keyword :
Black liquor Hydrogen production Sulfur transformation Supercritical water gasification
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GB/T 7714 | Lu, Libo , Wei, Wenwen , Liu, Fan et al. Sulfur transformation mechanism during supercritical water gasification of black liquor [J]. | FUEL , 2023 , 338 . |
MLA | Lu, Libo et al. "Sulfur transformation mechanism during supercritical water gasification of black liquor" . | FUEL 338 (2023) . |
APA | Lu, Libo , Wei, Wenwen , Liu, Fan , Ge, Zhiwei , Jin, Hui , Chen, Yunan et al. Sulfur transformation mechanism during supercritical water gasification of black liquor . | FUEL , 2023 , 338 . |
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Supercritical water gasification (SCWG) of coal has great application prospect for converting coal into hydrogen-rich gas efficiently and cleanly. However, the previous study on the reaction mechanism for SCWG of coal is relatively macroscopic rather than reflects the reaction essence deeply. The evolution of organic functional groups in Zhundong lignite (ZD), Hongliulin bitumite (HLL) and Ningxia anthracite (NX) during SCWG, as well as the correlation with gaseous products were analyzed quantitatively in this paper. It was found that the lower rank coal contained more free radicals and produced more H2 with SCW. H2 yield of the three types of coal exceeded 2 times the hydrogen content in coal at 800 degrees C. The organic functional groups evolve in 2-4 stages during SCWG process. The decomposition and gasification of organic functional groups mainly took place in low or medium temperature range. About 95% of C=O groups and 90% of aromatic C=C groups cracked and were gasified. Aromatic ether (Car-O) groups were formed in high temperature range. The reasonable functional relationship between the parameters of gaseous products and organic functional groups was established, providing a new approach to predict organic functional groups through gaseous products. This research may lay the foundation for further optimization design of reactor.(c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Keyword :
Coal rank Correlation Gasification Organic functional groups Supercritical water
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GB/T 7714 | Sun, Jingli , Luo, Kui , Feng, Huifang et al. Experimental investigation on organic functional groups evolution in hydrogen production process by coal gasification in supercritical water [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2023 , 48 (15) : 5887-5900 . |
MLA | Sun, Jingli et al. "Experimental investigation on organic functional groups evolution in hydrogen production process by coal gasification in supercritical water" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 48 . 15 (2023) : 5887-5900 . |
APA | Sun, Jingli , Luo, Kui , Feng, Huifang , Fan, Chao , Jin, Hui , Guo, Liejin . Experimental investigation on organic functional groups evolution in hydrogen production process by coal gasification in supercritical water . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2023 , 48 (15) , 5887-5900 . |
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Abstract :
Supercritical water upgrading heavy oil is a promising way to produce light oil and gas. To understand the reactions pathways and the role of supercritical water during the upgrading process, experiments were carried out in a batch reactor at 380-440 degrees C and reaction times up to 2900 min. The products were classified as gas, coke and liquid products which were further separated into saturates, aromatics, resins and asphaltenes. A kinetic model including aromatics and resins partially dissolved in both supercritical water phase and oil phase was developed. This model could fit experimental data well and interpret effects of supercritical water solubility for aromatics and resins on heavy oil upgrading process. Further, supercritical water upgrading process was divided into three stages: pre-induction primary cracking stage, post-induction primary cracking stage and gas -generation stage. This work provides an in-depth understanding of mechanism of heavy oil upgrading in su-percritical water.
Keyword :
Heavy oil upgrading Kinetic model Phase separation Supercritical water
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GB/T 7714 | Dong, Yu , Zhao, Qiuyang , Zhou, Yantao et al. Kinetic study of asphaltenes phase separation in supercritical water upgrading of heavy oil [J]. | FUEL PROCESSING TECHNOLOGY , 2023 , 241 . |
MLA | Dong, Yu et al. "Kinetic study of asphaltenes phase separation in supercritical water upgrading of heavy oil" . | FUEL PROCESSING TECHNOLOGY 241 (2023) . |
APA | Dong, Yu , Zhao, Qiuyang , Zhou, Yantao , Zheng, Lichen , Jin, Hui , Bawaa, Baercheng et al. Kinetic study of asphaltenes phase separation in supercritical water upgrading of heavy oil . | FUEL PROCESSING TECHNOLOGY , 2023 , 241 . |
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Realizing the harmless resource utilization of oily sludge is urgent for petroleum industry and of great signifi-cance for environmental management. The treatment of oily sludge was investigated using supercritical water gasification (SCWG) with a continuous fluidized bed reactor. The effect of operating parameters on gasification efficiency and gas yield without catalyst was tested, and then the influences of catalyst type (K2CO3 and Na2CO3) and concentrations (1-8 wt%) were systematically studied. The results indicated that a medium mass flow ratio and low feedstock concentration were beneficial for gas production. Alkali catalyst improved carbon gasification efficiency (CE) prominently, and Na2CO3 showed better performance due to its better stability. A maximum CE of 95.87% was achieved when 5 wt% Na2CO3 was added at 650 degrees C, 23 MPa with 5 wt% oily sludge concentration. Besides, according to XRD patterns of solid residues, Na2CO3 was more stable than K2CO3 during SCWG. SEM-EDX results also revealed that more K was migrated into solid residues than Na. The analysis of pore structure demonstrated that alkali catalyst promoted the evolution of pore structure, resulting in higher specific surface areas and total pore volumes. Na2CO3 has a more substantial destructive effect on solid matrix, causing the matrix structure to collapse and inhibiting pore structure development. The FTIR spectra of solid products exhibited a lower content of carbohydrates and aromatic structures than the initial oily sludge. NH4-N results demonstrated that SCWG was a potential green treatment process for oily sludge. This work can not only give an insight into the reaction mechanism of alkali catalytic gasification of oily sludge, but also help to guide the optimal design of reactor and the regulation of operating parameters.
Keyword :
Alkali catalyst Fluidized bed reactor Oily sludge Supercritical water gasification
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GB/T 7714 | Li, Linhu , Wang, Gaoyun , Li, Xujun et al. Experimental study on alkali catalytic gasification of oily sludge in supercritical water with a continuous reactor [J]. | JOURNAL OF ENVIRONMENTAL MANAGEMENT , 2023 , 327 . |
MLA | Li, Linhu et al. "Experimental study on alkali catalytic gasification of oily sludge in supercritical water with a continuous reactor" . | JOURNAL OF ENVIRONMENTAL MANAGEMENT 327 (2023) . |
APA | Li, Linhu , Wang, Gaoyun , Li, Xujun , Wang, Le , Zhang, Jiawei , Cheng, Ke et al. Experimental study on alkali catalytic gasification of oily sludge in supercritical water with a continuous reactor . | JOURNAL OF ENVIRONMENTAL MANAGEMENT , 2023 , 327 . |
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Abstract :
In the heterogeneous photocatalytic reaction systems, the evolution of bubbles on the catalyst surface is a complex process that depends on multiple factors, such as the solid-liquid interface structure, solution properties of the reaction system, and multiphysics interactions, and directly affects energy and mass transport processes. This study investigated the multiphysics distribution around a bubble and the bubble detachment characteristics on the surface of a TiO2 photoelectrode during photoelectrocatalytic water splitting. The bubble diameter had an effect on the distribution of the light field in the system, affecting the temperature and flow distributions of the electrolyte around the bubble. Marangoni convection was induced by the inhomogeneous temperature distribution along the bubble interface, which enhanced the heat and mass transfer near the reaction site. It was also demonstrated that an increase in laser power increased Marangoni convection on the bubble surface, thus delaying bubble detachment. A force model for predicting the bubble detachment diameter that considered the coupling effect between the light, temperature, and flow fields was developed. The predicted bubble detachment diameters agreed well with the experimental results within an error of +/- 10%.
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GB/T 7714 | Cao, Zhenshan , Feng, Yuyang , Zhang, Bo et al. Distribution Characteristics of Multiphysics around the Bubble on the Surface of Photoelectrode [J]. | JOURNAL OF THE ELECTROCHEMICAL SOCIETY , 2022 , 169 (12) . |
MLA | Cao, Zhenshan et al. "Distribution Characteristics of Multiphysics around the Bubble on the Surface of Photoelectrode" . | JOURNAL OF THE ELECTROCHEMICAL SOCIETY 169 . 12 (2022) . |
APA | Cao, Zhenshan , Feng, Yuyang , Zhang, Bo , Xu, Qiang , Wang, Yechun , Guo, Liejin . Distribution Characteristics of Multiphysics around the Bubble on the Surface of Photoelectrode . | JOURNAL OF THE ELECTROCHEMICAL SOCIETY , 2022 , 169 (12) . |
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Supercritical multi-component thermal fluid (SMTF) generation technology is vastly promising for the application of offshore heavy oil recovery. The first step of the novel technology is hydrogen production by supercritical water gasification (SCWG). And oilfield wastewater can be used directly for SMTF generation as a toxic waste of heavy oil recovery. In this paper, crude oil was used as a model compound for oilfield wastewater. Experiments were conducted at a pressure of 25 MPa, the temperature of 600-700 degrees C, the residence time of 2-30 min, the feedstock concentration of 2-8 wt%, and with Na2CO3 as a catalyst. The results showed that the gas yield and carbon gasification efficiency (CE) were improved under the catalysis of Na2CO3. The increased reaction temperature and prolonged residence time were both beneficial for high CE. The most abundant gaseous product was H-2 and the maximum CE was 96.12%. The intermediate products from SCWG were analyzed using the lumped parameter method to establish the reaction pathways and kinetics model. This quantitative kinetics model was developed to describe the gaseous products, which consist of H-2, CO, CH4, and CO2. The model turned out to be robust by the experimental results. This work would be of great value to reveal the mechanism of SMTF generation technology.
Keyword :
Kinetics Oilfield wastewater Reaction pathways Supercritical multi-component thermal fluid Supercritical water gasification
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GB/T 7714 | Peng, Zhiyong , Rong, Siqi , Xu, Jialing et al. Reaction pathways and kinetics for hydrogen production by oilfield wastewater gasification in supercritical water [J]. | FUEL , 2022 , 314 . |
MLA | Peng, Zhiyong et al. "Reaction pathways and kinetics for hydrogen production by oilfield wastewater gasification in supercritical water" . | FUEL 314 (2022) . |
APA | Peng, Zhiyong , Rong, Siqi , Xu, Jialing , Jin, Hui , Zhang, Jiawei , Shang, Fei et al. Reaction pathways and kinetics for hydrogen production by oilfield wastewater gasification in supercritical water . | FUEL , 2022 , 314 . |
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Supercritical water gasification (SCWG) of oily sludge is a potential handling method for resource utilization and pollution reduction. Heavy metals (HMs) in oily sludge were assessed due to their threat to human health and environmental safety. This work investigated the distribution of four HMs (Cu, Zn, Ni and Cr) under different reaction conditions (550-700 degrees C, 1-60 min). The concentrations of HMs in liquid residues (LRs) decreased continuously at higher temperatures and longer residence times except for Ni. Besides, the concentrations of HMs in solid residues (SRs) increased after SCWG except for Zn, and they varied slightly under different conditions. Then, HMs in LRs and SRs were evaluated in terms of Nemerow index, geo-accumulation index and potential ecological risk. The results indicated that the pollution risks of HMs in LRs were minimum at 650 degrees C and 30 min, while that in SRs changed little. When Na2CO3 was added, pollution risks changed slightly, but nearly complete stabilizations of Cu, Zn and Cr (96.2%, 84.2% and 98.6%) were achieved at 600 degrees C. Adding Na2CO3 promoted the formation of aluminosilicate to combine with HMs and enhanced their stabilization notably. This work may demonstrate a promising clean way for oily sludge utilization and HMs stabilizing.
Keyword :
Heavy metals Oily sludge Stabilization Supercritical water gasification
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GB/T 7714 | Li, Linhu , Cao, Wen , Peng, Pai et al. Distribution, risk assessment and stabilization of heavy metals in supercritical water gasification of oily sludge [J]. | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2022 , 168 : 591-600 . |
MLA | Li, Linhu et al. "Distribution, risk assessment and stabilization of heavy metals in supercritical water gasification of oily sludge" . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION 168 (2022) : 591-600 . |
APA | Li, Linhu , Cao, Wen , Peng, Pai , Wang, Gaoyun , Liu, Shi , Jin, Hui et al. Distribution, risk assessment and stabilization of heavy metals in supercritical water gasification of oily sludge . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2022 , 168 , 591-600 . |
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The photochemical system, which utilizes only solar energy and H2O/CO2 to produce hydrogen/carbon-based fuels, is considered a promising approach to reduce CO2 emissions and achieve the goal of carbon neutrality. To date, numerous photochemical systems have been developed to obtain a viable solar-to-fuel production system with sufficient energy efficiency. However, more effort is still needed to meet the requirements of industrial implementation. In this review, we systematically discuss a typical photochemical system for solar-to-fuel production, from classical theories and fundamental mechanisms to raw material selection, reaction condition optimization, and unit device/system advancement, from the viewpoint of ordered energy conversion. State-of-the-art photochemical systems, including photocatalytic, photovoltaic-electrochemical, photoelectrochemical, solar thermochemical, and other emerging systems, are summarized. We highlight the existing bottlenecks and discuss the developing trend of this technology. Finally, optimization strategies and new opportunities are proposed to enhance photochemical systems with higher energy efficiency.
Keyword :
Carbon-based fuels Hydrogen Photochemical Solar energy
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GB/T 7714 | Liu, Ya , Wang, Feng , Jiao, Zihao et al. Photochemical Systems for Solar-to-Fuel Production [J]. | ELECTROCHEMICAL ENERGY REVIEWS , 2022 , 5 (3) . |
MLA | Liu, Ya et al. "Photochemical Systems for Solar-to-Fuel Production" . | ELECTROCHEMICAL ENERGY REVIEWS 5 . 3 (2022) . |
APA | Liu, Ya , Wang, Feng , Jiao, Zihao , Bai, Shengjie , Qiu, Haoran , Guo, Liejin . Photochemical Systems for Solar-to-Fuel Production . | ELECTROCHEMICAL ENERGY REVIEWS , 2022 , 5 (3) . |
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Organic-rich shale resources are large reserves with high hydrocarbon generation potential but are difficult to exploit due to their high solid kerogen content. Supercritical water conversion was proposed as an alternative method to convert kerogen into oil and gas because supercritical water has favorable solubility, dispersion, and reactivity. In this study, Chang 7 shale containing a high TOC content of 15.11%, type II kerogen, and low Ro of 0.36-0.38% in the Ordos basin was taken as a typical example of organic-rich shale with low maturity. A series of experiments at the temperatures of 300-650 degrees C and a pressure of 25 Mpa were carried out to test the feasibility, and the shale conversion performance was analyzed from three perspectives, hydrocarbon generation of kerogen, the effect of inorganic minerals, and shale pore evolution. The optimum oil and gas yields were, respectively, found to be 352.1 mg (g TOC)(-1) (g TOC refers to total organic carbon mass in shale) at 380 degrees C and 852.0 mL (g TOC)(-1) at 650 degrees C. Compared with pyrolysis in the aluminium retort, supercritical water conversion raised the oil yield at the same temperature (171.4 mg (g TOC)(-1) at 380 degrees C) or reduced the temperature with the same yield (346.8 mg (g TOC)(-1) at 520 degrees C). Chang 7 shale minerals as a whole increased the oil yield by 34.2% at 380 degrees C but had a negligible effect on gas generation. Among them, the carbonate (dolomite) promoted oil generation but inhibited gas generation, while the silicates (feldspar, quartz, and clay) did the opposite, and the pyrite favored both oil and gas generation. Additionally, the supercritical water conversion significantly increased the shale pore volume and specific surface area because the hydrocarbon generation of kerogen produced many nanopores with slit-like shapes and diameters of 50-5000 nm. This paper provides an in-depth understanding of sub- and supercritical water conversion of low-maturity shale for oil and gas production.
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GB/T 7714 | Zhao, Qiuyang , Dong, Yu , Zheng, Lichen et al. Sub- and supercritical water conversion of organic-rich shale with low-maturity for oil and gas generation: using Chang 7 shale as an example [J]. | SUSTAINABLE ENERGY & FUELS , 2022 , 7 (1) : 155-163 . |
MLA | Zhao, Qiuyang et al. "Sub- and supercritical water conversion of organic-rich shale with low-maturity for oil and gas generation: using Chang 7 shale as an example" . | SUSTAINABLE ENERGY & FUELS 7 . 1 (2022) : 155-163 . |
APA | Zhao, Qiuyang , Dong, Yu , Zheng, Lichen , Xie, Tian , Bawaa, Baercheng , Jin, Hui et al. Sub- and supercritical water conversion of organic-rich shale with low-maturity for oil and gas generation: using Chang 7 shale as an example . | SUSTAINABLE ENERGY & FUELS , 2022 , 7 (1) , 155-163 . |
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Supercritical water gasification (SCWG) is a promising clean technology for coal utilization due to high chemical reactivity and no tar emission. However, the wall-type heat exchange in the SCWG system demands a large heating surface area and an extreme high-temperature heat source. This paper puts forward an optimized design, namely direct mass transfer, in which the final product gas is partially recycled back into the gasification reactor to supplement the gasification agent and provide sensible heat energy. A whole system simulation was established to analyze the mass flow and exergy efficiency in the reference design and the optimized design. The process analysis shows that the optimized design has higher exergy efficiency (85.6%) than that (72.5%) of the reference design. In the optimized system, direct mass transfer significantly alters the mass flow and exergy flow, with less influent water (33.3%), less heat transfer rate (30.5%), and less oxygen consumption (51.5%). Furthermore, sensitivity analysis shows that increasing circulation ratio, feedstock concentration, and preheating temperature can reduce oxygen consumption and improve gas output and efficiency. The study indicates that direct mass transfer has the potential superiority to solve the challenge of heat integration and facilitate the application of the industrial-scale SCWG system.
Keyword :
Direct mass transfer Exergy efficiency Heat integration Sensitivity analysis Supercritical water gasification
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GB/T 7714 | Guo, Shenghui , Meng, Fanrui , Peng, Pai et al. Thermodynamic analysis of the superiority of the direct mass transfer design in the supercritical water gasification system [J]. | ENERGY , 2022 , 244 . |
MLA | Guo, Shenghui et al. "Thermodynamic analysis of the superiority of the direct mass transfer design in the supercritical water gasification system" . | ENERGY 244 (2022) . |
APA | Guo, Shenghui , Meng, Fanrui , Peng, Pai , Xu, Jialing , Jin, Hui , Chen, Yunan et al. Thermodynamic analysis of the superiority of the direct mass transfer design in the supercritical water gasification system . | ENERGY , 2022 , 244 . |
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