JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Meilu Hao,Peng Liang,Miaomiao Tian,Songze Li,Yue Gao,Yaqing Zhang,Xizhuang Qin,Wenrui Zhang,Tiantian Jiao
To efficiently utilize the oxygenated structures in lignite and obtain value-added oxygenated compounds, this study proposes a low carbon cascading utilization of Zhaotong lignite (ZT) through thermal dissolution and pyrolysis. The selectivity of ethanol (ET), tetrahydrofuran (THF) and ethyl acetate (EA) for oxygenated compounds in thermal dissolution, and the enrichment of thermal dissolution-pyrolysis on oil phases were investigated. The results show that sequential thermal dissolution is selective for different oxygenated compounds in ZT. ET shows selectivity for esters at 350 °C-2 MPa and for phenols at 350 °C-6 MPa. THF and EA are selective for naphthols and esters at 350 °C-6 MPa, respectively. Compared with the single process of thermal dissolution or pyrolysis, thermal dissolution-pyrolysis can significantly increase the oil phases yield with high value-added, in which ET, THF and EA increase the oil phase yields by 24.81 wt%, 13.66 wt% and 7.90 wt%, respectively. In particular, 59.15 wt% of the oxygen is distributed in light oil, and 9.79 % phenols as well as 1.56 % esters are enriched into light oil during thermal dissolution-pyrolysis process of ET. High value-added oxygenated compounds can be selectively enriched by appropriate solvents, at the same time, the quality of pyrolysis tar can be improved and the carbon emissions could be reduced.
研究领域:
化学工程
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能源科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 10
·1181
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IF 4.501
Da Song,Yan Lin,Kun Zhao,Zhen Huang,Fang He,Ya Xiong
CO2resourceful utilization contributes to the goal of carbon neutrality. Chemical Looping Dry Reforming (CLDR) has attracted significant attention as a method for converting CO2to CO. NiFe2O4oxygen carrier (OC) is found to be a potential material for CLDR. However, the migration process of lattice oxygen, which are critical for the conversion of CO2to CO, was not extensively investigated. In this study, the reduction and oxidation degrees of the NiFe2O4were finely modulated in a thermogravimetric analyzer. The lattice oxygen migration mechanism of the NiFe2O4in redox cycles was characterized by means of X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and in-situ Raman. The novelty of this paper is clarifying the release-uptake paths of lattice oxygen during CO2resourceful utilization. The result indicates that the concentration gradient between the surface and the bulk drives the diffusion of lattice oxygen. The stabilization of surface lattice oxygen content is attributed to the rapid migration of O anion, which is closely associated with the movement process of Ni particles inward and outward through the spinel bulk. In addition, a highly reactive chemical reaction interface consisting of lattice oxygen and the corresponding metal atoms is always present on the surface of the oxygen carrier and is confirmed by an in-situ Raman and XPS during the whole process of CLDR. The results of this paper offer reference and basis for further development and design of CLDR using spinel OC.Keywords:chemical looping (CL);oxygen carrier (OC);CO2splitting;lattice oxygen;NiFe2O4
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
LAND DEGRADATION & DEVELOPMENT
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2025
·
IF 3.7
Qiuyue Zhang,Yi Tang,Yanjiao Wang,Pengfei Cheng,Lianghui Li,Babar Iqbal,Tingting Zhao,Ruoyu Guo,Xiaojun Zheng,Guanlin Li,Daolin Du
Microplastics and antibiotics are emerging pollutants that accumulate extensively in soils, both exerting adverse effects on soil ecosystems. The mechanisms underlying the combined effects of microplastics and antibiotics on soil microbial metabolism remain insufficiently understood. Therefore, we evaluated the individual and combined effects of different types of microplastics (non-degradable polyethylene and biodegradable polylactic acid) and an antibiotic (oxytetracycline) on soil microbial metabolism characteristics. Our results showed that the microbial community was primarily limited by nitrogen under either microplastics or antibiotics treatments; whereas it was limited by phosphorus under the combined treatments. All treatments, except for the non-biodegradable microplastic treatment, significantly alleviated carbon limitation in the microbial community ( p < 0.01), with the effect being particularly pronounced under combined treatments involving both types of microplastics and antibiotics. Notably, both individual and combined treatments significantly increased the microbial carbon use efficiency ( p < 0.05). The effects of microplastics on microbial metabolism were influenced by both the type of microplastics and their interaction with antibiotics, highlighting the complex nature of these combined environmental pollutants. This study provided an empirical basis for understanding the individual exposure and co-exposure to biodegradable/non-biodegradable microplastics and antibiotics on soil microbial metabolism.
研究领域:
环境科学
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微生物学
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生态学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2020
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IF 5.578
Hang Zhang,Shimin Kang,Jietai Li,Zhilin Li,Jie Chang,Yongjun Xu,Gaoqing Max Lu,Chenghua Sun
Fuel production from biomass offers a low-carbon strategy to address the global challenge of climate change associated with carbon emission. Novel technique with high carbon- and energy-recovery from biomass has been pursued for decades, but rarely achieved. Here we demonstrate the near zero-waste production of high-quality biofuels from poly(3-hydroxybutyrate), a biofeedstock widely accumulated in microorganisms, under mild temperature (200 °C), with 99% carbon utilization and 91.5% energy recovery. Products are dominated by easy-to-use alkanes, butyrates and butanol. This technique paves the way for green production of biofuels from bioderived feedstocks.
研究领域:
生物化学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Ke Wang,Jie Chen,Tianyu Wang,Jie Hong,Pengfei Zhao,Edward J. Anthony
Capture and conversion of CO 2 from optimal-scenarios into fuels or chemicals provide a viable solution to combat climate change in reducing greenhouse gas emissions. Here, we propose and experimentally demonstrate that synergistic integration (Catalytic calcium-looping (CaL) gasification of biochar) can realize the capture and in situ conversion of CO 2 . Thermodynamic and kinetic estimations, catalytic conversion and cyclic tests and microstructure characterizations showed that by using a mixture of limestone and K 2 CO 3 -impregnated biochar, calcination fully coupled with the reverse Boudouard reaction can shift thermodynamic equilibrium and simultaneously induce the synergetic catalysis between CaCO 3 and K 2 CO 3 , allowing for accelerating decarbonation kinetics, enhancing CO yield and maintaining stable cyclic CO 2 conversion at lower temperatures (850 °C), as compared to the individual CaL and gasification processes. Theoretical calculations further revealed that the activation energy barriers for the monatomic C-assisted CO 2 dissociation were lower than its desorption energy for CO 2 on the K-doped CaO surface, demonstrating superior conversion reactivity. Importantly, the process is demonstrated in terms of practical scalability using a renewable and cost-effective reductant (biochar), a cheap catalyst (K 2 CO 3 ) and inexpensive natural CO 2 sorbents (limestone and dolomite) in an energy-efficient manner, therefore opening a unique direction for net-negative emission for large CO 2 stationary sources eliminating the need for sequestration.
研究领域:
能源与环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Jian Fang,Zhi-Qiang Wang,Xinjia Wei,Yuan Ma,Honghui Gong,Xue-Qing Gong,Zhenshan Hou
The N-formylation reaction of various amines with CO2 is a promising method to utilize CO2 for the production of high value-added chemicals. Herein, an efficient Ru catalyst system consisting of Ru complex ([PPN][Ru(CO)3Cl3]) and the ionic liquid 1-butyl-3-methylimidazolium hydrogen phosphate ([Bmim]2[HPO4]), has been developed for the N-formylation reaction. Activity evaluation demonstrated that the catalyst system exhibited good to excellent yields of formamides under very mild conditions with the assistance of ionic liquids (ILs). Furthermore, the catalyst system could be reused at least five times with a slight loss of activity in N-formylmorpholine production. Further characterization by 1H nuclear magnetic resonance (NMR), 13C NMR, and density functional theory (DFT) calculations showed that the ILs ([Bmim]2[HPO4]) could facilitate the adsorption of CO2 by a concerted action of both cations and anions of the ILs to form phosphorus carbonate intermediate, thus effectively promoting the reaction. DFT calculations demonstrated that the formation of Ru–H was the first step, and then the CO2 absorbed by [Bmim]2[HPO4] inserted directly into Ru–H by cooperating with the Ru sites to form HCOO– species. After that, formate species dissociated from Ru catalysts and dehydrated to form formamides by the catalytic action of Ru complex and the basic IL.
研究领域:
化学工程
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催化化学
✓ 已验证
DOI
高影响因子
ORGANOMETALLICS
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2023
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IF 2.8
Yanru Zhang,Jingjing Zhang,Ying Wang,Yang Li,Jun He,Yanyan Wang,Longbo Zhang,Zhenpeng Wang,Qingli Qian,Buxing Han
Synthesis of basic C2+ chemicals using CO2 and H2 is very promising. Herein, we present a protocol for the synthesis of different carboxylic acids by the reaction of ketones or aldehydes with CO2 and H2. The catalytic system consisted of the IrCl3 catalyst, LiI promoter, and acetic acid solvent. The yield can reach 52.9% based on the cyclohexanone substrate which can be derived from biomass. Various Cn ketones and aldehydes could be used as a substrate in the reaction, where the corresponding Cn+1 carboxylic acids were obtained. According to the mechanistic study, the reaction involved substrate conversion, reverse water–gas shift (RWGS) reaction, and carbonylation. This strategy provides an optional way of carboxylic acid production and CO2 utilization.
研究领域:
有机化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2024
·
IF 1.3
Wenhui Dong,Xinyuan Sun,Qianqian Niu,Yun Zhu,Baokang Jin
Phenylacetic acid derivatives, including 1-naphthaleneacetic acid, hold crucial applications in various domains. Traditional synthesis methods often involve intricate steps or the use of expensive and polluting heavy metal catalysts. This paper presents an electrochemical approach for efficiently producing valuable compounds like 1-naphthaleneacetic acid and other phenylacetic acid analogs through the reduction of benzyl halides, such as 1-chloromethyl naphthalene, in the presence of CO 2 . At the same time as preparing phenylacetic acid, the resource utilization of CO 2 is realized. Six kinds of carboxy analogs were synthesized by potentiostatic electrolysis of benzyl halides in acetonitrile with CO 2 as a co-reactant and tetraethyl ammonium tetrafluoroborate as an electrolyte. The electrochemical reduction products were confirmed structurally through NMR, mass spectrometry, and other techniques. The Faraday electrolysis efficiencies ranged from 82 % to 94 %, with 72.5–92.9 % conversions. The study delves into the electron transfer mechanism using cyclic voltammetry and in situ FT-IR spectroelectrochemistry. The reduction process on silver electrodes under a CO 2 atmosphere was identified as an irreversible two-electron process, generating a monovalent anion that attacks CO 2 to yield the respective carboxyl analogs.
研究领域:
有机化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Xinyuan Sun,Dan Li,Qianqian Niu,Yan Liu,Dandan Zhang,Longjiu Cheng,Baokang Jin
Cyclic azobenzenes are capable of undergoing reversible cis-trans isomerization upon visible light irradiation, making them promising candidates as molecular photoswitches for applications in biological systems. However, their synthesis remains challenging due to their unique structural features. In this study, two eight-membered cyclic azobenzenes, namely 12H-dibenzo[b,f][1,4,5]thiadiazocine ( 13 ) and 12H-dibenzo[b,f][1,4,5] oxadiazocine ( 14 ), were synthesized through electrochemical reduction of 2’-nitrobenzyl-2-nitrophenyl-sulfide ( 1 ) and 1-nitro-2-((2’-nitrobenzyl)oxy)benzene ( 2 ), respectively, in the presence of CO₂. The synthesis yielded high conversion rates ( 13 : 85.98%, 14 : 93.76%). Using in situ infrared spectroscopy, NMR, and MS, detailed reduction mechanisms were elucidated, revealing an irreversible 8-electron transfer process and CO₂ involvement in a four-step reaction pathway. UV-Vis spectroscopic analysis showed that both 13 and 14 undergo trans-to-cis isomerization upon exposure to yellow (520 nm) or red (630 nm) light, in agreement with theoretical calculations. Additionally, S0→S1 excitations of both cis and trans isomers are predominantly governed by n→π* transitions. It is found that the cis conformation of compounds 13 and 14 is more stable than the trans conformation. Under yellow or red light irradiation, they undergo rapid trans-to-cis isomerization. No photochemical fatigue was observed in the cyclic experiments at room temperature, indicating their excellent photostability and potential application in photopharmacology. This work offers a sustainable strategy for the synthesis of cyclic azobenzenes and CO₂ capture.
研究领域:
有机化学
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材料科学
·
光化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Industrial and Engineering Polymer Research
·
2019
·
IF 0
Jiaxiang Qin,Junqiao Jiang,Shuxian Ye,Jiaxin Liang,Youji Tao,Shuanjin Wang,Dongmei Han,Min Xiao
As carbon dioxide (CO 2 ) is an inexpensive, abundant, sustainable and green carbonyl resource, its utilization to produce value-added chemicals and polymeric materials has attracted much more attention. In this work, a novel CO 2 route polyurea (PUa) was synthesized. The chemical composition, molecular structure, and aggregation structure of polyurea has been confirmed by 1 H-NMR, HMBC-NMR, DSC, TG, MALDI-TOF MS and POM. The result from POM shows that polyurea gives out a spherulitic morphology, exhibited a typical black cross pattern formed by many concentric circles with different light and shade. Moreover, shape memory polymers of polyurea-multiblock-poly(propylene carbonate) (PUa- mb -PPCs) with a M n nearly 4.72 × 10 4 Da and a polydispersity index (PDI) of 1.51–1.64 were synthesized by chain extension of the polyurea with CO 2 derived poly(propylene carbonate) diols (PPC-OH). The PUa- mb -PPCs possess high strength and elasticity because the crystallinity formed by polyurea and amorphous region from PPC. Notably, excellent shape memory effect (SME) is observed in shape thermomechanical testing. The present work provides a simple and renewable process for the synthesis of CO 2 -copolymer with multiblock structure, opening a new route for preparation of functional polymeric materials from carbon dioxide conversion.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
APPLIED CATALYSIS A-GENERAL
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2019
·
IF 4.63
Yongdong Chen,You Yang,Shanli Tian,Zhongbin Ye,Qiang Tang,Lin Ye,Gao Li
Greenhouse effect raised by the carbon dioxide emissions has become a pivotal resolved issue at present. The direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol is one of infusive green pathways. In this study, a novel CuNi alloy nanoparticles encapsulated in a thermal stable triphenylphosphine porous organic polymers (POP-PPh 3 ), Cu x Ni y @POP-PPh 3 catalysts, is synthesized and then explored in the direct DMC synthesis reactions. The Cu x Ni y @POP-PPh 3 catalysts are fully characterized by a series of techniques, such as transmission electron microscopy (TEM) with energy-dispersive spectroscopy (EDS), X-ray diffraction (XRD), N 2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy (XPS), and hydrogen temperature programmed reduction (H 2 -TPR). TEM images show the CuNi particles are around 7 nm, and XPS analyses demonstrate the alloy particles comprise of a metallic (CuNi) 0 core and a thin Ni 2 O 3 surface. The Cu x Ni y @POP-PPh 3 catalysts, fixed into a honeycomb ceramic to give a monolithic catalyst, show an excellent catalytic performance (a 10.5% methanol conversion with an 80% DMC selectivity) during the direct DMC synthesis reactions in a fixed bed reactor. The high catalytic performance over Cu x Ni y @POP-PPh 3 catalysts is mainly attributed to the pore structure of POP-PPh 3 , uniform distribution of alloy nanoparticles, and the unique performance of the monolithic catalyst ( e.g ., removing by-product of water in time).
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Sustainability
·
2023
·Vol. 6
·期 6
·712-719
·
IF 27.6
Sun Bo,Zhang Jie,Wang Maolin,Yu Shixiang,Xu Yao,Tian Shuheng,Gao Zirui,Xiao Dequan,Liu Guosheng,Zhou Wu,Wang Meng,Ma Ding
Biodegradable polyesters such as polylactic acid are promising alternatives to conventional plastics as they do not accumulate in the environment upon disposal. However, their biodegradation leads to CO 2 emissions. Alternatively, waste biodegradable polyesters could serve as a carbon source for the production of value-added chemicals. Valorization of waste biodegradable polyesters not only avoids CO 2 emissions during their biodegradation but also achieves sustainable carbon use. Here, we report a two-step catalytic process to convert polylactic acid waste into methyl methacrylate, a key building-block molecule. Polylactic acid is first transformed into methyl propionate with near-quantitative yields (conversion >99%, selectivity 98%) over the α-MoC catalyst in methanol solution, which is followed by reacting the obtained methyl propionate with formaldehyde to produce methyl methacrylate with a conversion of 81% and selectivity of 90%. This study opens up a new path for managing end-of-life biodegradable polyester plastics and contributing to a circular economy.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）