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Low-concentration and multi-component NMHCs capture from oil field exhaust using porous ZIF-8/iso-hexadecane slurry

Green Chemical Engineering 2024年第2期5卷 245-256页

作者： Kun Li Han Tang Jin Cai Chun Deng Bei Liu Yunlei Peng Changyu Sun Guangjin Chen state key laboratory of heavy oil processing China University of PetroleumBeijing102249China

Non-methane hydrocarbons(NMHCs)are a common type of volatile organic compounds(VOCs)pollutant in the petrochemical industry and have attracted widespread attention because of their adverse health effects and environmental impacts.In this paper,we report a new porous slurry formed with zeolitic imidazolate framework-8(ZIF-8)and iso-hexadecane to capture the low-concentration and multi-component NMHCs(mainly ethane(C_(2)H_(6)),propane(C_(3)H_(8)),and n-butane(n-C_(4)H_(10)))from the oil field exhaust.The sorption capacity of C_(2)H_(6)in the slurry is significantly higher than that of nitrogen(N_(2))and methane(CH_(4)).Moreover,the slurry demonstrated a clear advantage for C_(2)H_(6)over N_(2)and CH_(4)in competitive adsorption through the pressure-drop curves.In the NMHCs capture experiments,the C_(3)H_(8)and n-C_(4)H_(10)concentrations after purification can be reduced to below 100 ppm,while the C_(2)H_(6)concentration can reach approximately 180 ppm.More encouragingly,in the breakthrough tests,the slurry exhibits a perfect kinetic separation selectivity for multi-component NMHCs.Furthermore,to avoid structural collapse of ZIF-8 material during long-term use in acidic and wet environments,a certain amount of 2-methylimidazole was retained in the slurry as a protective agent in the material synthesis process.In this way,the ZIF-8 materials in the slurry can retain the stable characteristic structure in an aqueous and acidic environment and keep the capture capacity for NMHCs without degradation.We believe the porous ZIF-8/iso-hexadecane slurry is a promising capture agent for low-concentration and multi-component NMHCs with strong purification capacity and stability.

关键词： VOCs capture NMHCs capture MOFs ZIF-8 Porous slurry

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Internal Polarization Field Induced Hydroxyl Spillover Effect for Industrial Water Splitting Electrolyzers

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Nano-Micro Letters 2024年第2期16卷 438-449页

作者： Jingyi Xie Fuli Wang Yanan Zhou Yiwen Dong Yongming Chai Bin Dong state key laboratory of heavy oil processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580People’s Republic of China

The formation of multiple oxygen intermediates supporting efficient oxygen evolution reaction(OER)are affinitive with hydroxyl adsorption.However,ability of the catalyst to capture hydroxyl and maintain the continuous supply at active sits remains a tremendous challenge.Herein,an affordable Ni2P/FeP2 heterostructure is presented to form the internal polarization field(IPF),arising hydroxyl spillover(HOSo)during OER.Facilitated by IPF,the oriented HOSo from FeP2 to Ni2P can activate the Ni site with a new hydroxyl transmission channel and build the optimized reaction path of oxygen intermediates for lower adsorption energy,boosting the OER activity(242 mV vs.RHE at 100 mA cm-2)for least 100 h.More interestingly,for the anion exchange membrane water electrolyzer(AEMWE)with low concentration electrolyte,the advantage of HOSo effect is significantly amplified,delivering 1 A cm^(-2)at a low cell voltage of 1.88 V with excellent stability for over 50 h.

关键词： Hydroxyl spillover effect Internal polarization field Heterostructure Oxygen reduction reaction Anion exchange membrane water electrolysis

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Fabrication of highly effective electrodes for iron chromium redox flow battery

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Nano Research 2024年第5期17卷 3988-3996页

作者： Yingchun Niu Chao Guo Yinping Liu Guangfu Wu Tianhang Zhou Fangang Qu Ziji Yang Ali Heydari Chunming Xu Quan Xu state key laboratory of heavy oil processing China University of Petroleum(Beijing)Beijing 102249China

Iron-chromium redox flow batteries(ICRFBs)have emerged as promising energy storage devices due to their safety,environmental protection,and reliable performance.The carbon cloth(CC),often used in ICRFBs as the electrode,provides a suitable platform for electrochemical processes owing to its high surface area and interconnected porous structure.However,the CC electrodes have issues,such as,insufficient electron transfer performance,which limits their industrial application.Here,we employed silicic acid etching to carve dense nano-porous structures on the surface of CC electrodes based on the favorable design of ICRFBs and the fundamental principles of electrode polarization losses.As a result,we developed a multifunctional carbon cloth electrode with abundant vacancies,notably enhancing the performance of the battery.The fabricated electrode showcased a wealth of defect sites and superior electronic transport properties,offering an extensive and effective reaction area for rapidly flowing electrolytes.With an electrode compression ratio of 40%and the highest current density in ICRFBs so far(140 mA·cm^(-2)),the battery achieved the average energy efficiency of 81.3%,11.24%enhancement over the previously published work.Furthermore,throughout 100 charge-discharge cycles,the average energy efficiency degradation was negligible(~0.04%),which has the potential to become the most promising candidate for large-scale and long-term electrochemical energy storage applications.

关键词： iron chromium redox flow battery electron carbon cloth defect site density functional theory(DFT)calculation

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Rate-limiting factors in hydrate decomposition through depressurization across various scales:A mini-review

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Chinese Journal of Chemical Engineering 2024年第3期67卷 206-219页

作者： Xian Sun Peng Xiao Qinfeng Shi Lingban Wang Zhenbin Xu Yuhao Bu Xiaohui Wang Yifei Sun Changyu Sun Guangjin Chen state key laboratory of heavy oil processing China University of Petroleum(Beijing)Beijing 102249China Jining University Jining 273115China

Natural gas hydrate is an energy resource for methane that has a carbon quantity twice more than all traditional fossil fuels combined.However,their practical application in the field has been limited due to the challenges of long-term preparation,high costs and associated risks.Experimental studies,on the other hand,offer a safe and cost-effective means of exploring the mechanisms of hydrate dissociation and optimizing exploitation conditions.Gas hydrate decomposition is a complicated process along with intrinsic kinetics,mass transfer and heat transfer,which are the influencing factors for hydrate decomposition rate.The identification of the rate-limiting factor for hydrate dissociation during depressurization varies with the scale of the reservoir,making it challenging to extrapolate findings from laboratory experiments to the actual exploitation.This review aims to summarize current knowledge of investigations on hydrate decomposition on the subject of the research scale(core scale,middle scale,large scale and field tests)and to analyze determining factors for decomposition rate,considering the various research scales and their associated influencing factors.

关键词： Gas hydrate Rate-limiting factors Research scale Depressurization Decomposition

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Synergistic effects and kinetics analysis for co-pyrolysis of vacuum residue and plastics

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Frontiers of Chemical Science and Engineering 2024年第5期18卷 71-81页

作者： Chao Wang Xiaogang Shi Aijun Duan Xingying Lan Jinsen Gao Qingang Xiong state key laboratory of heavy oil processing China University of Petroleum-BeijingBeijing 102249China state key laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510640China

This study utilizedathermogravimetric analyzer to assess the thermal decomposition behaviors and kinetics properties of vacuum residue(VR)and low-density polyethylene(LDPE)polymers.The kinetic parameters were calculated using the Friedman technique.To demonstrate the interactive effects between LDPE and VR during the co-pyrolysis process,the disparity in mass loss and mass loss rate between the experimental and calculated values was computed.The co-pyrolysis curves obtained through estimation and experimentation exhibited significantdeviations,whichwerei influencedby temperature and mixing ratio.A negative synergistic interaction was observed between LDPE and VR,although this inhibitory effect could be mitigated or eliminated by reducing the LDPE ratio in the mixture and increasing the co-pyrolysistemperature.Theco-pyrolysisprocess resulted in a reduction in carbon residue,which could be attributed to the interaction between LDPE and the heavy fractions,particularly resin and asphaltene,present in VR.These findings align with the pyrolysis behaviors exhibited by the four VR fractions.Furthermore,it was observed that the co-pyrolysis process exhibited lower activation energy as the VR ratio increased,indicating a continuous enhancement in the reactivity of the mixed samples during co-pyrolysis.

关键词： co-pyrolysis heavy residual oil polyethylene thermogravimetric analysis synergistic effects

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Ca and Sr co-doping induced oxygen vacancies in 3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts for boosting low-temperature oxidative coupling of methane

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Journal of Energy Chemistry 2024年第4期91卷 331-344页

作者： Tongtong Wu Yuechang Wei Jing Xiong Yitao Yang Zhenpeng Wang Dawei Han Zhen Zhao Jian Liu state key laboratory of heavy oil processing China University of PetroleumBeijing 102249China key laboratory of Optical Detection Technology for oil and Gas China University of PetroleumBeijing 102249China

It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.

关键词： 3DOM catalysts Ca ions Sr ions Low-temperature oxidative couplingof methane Oxygen vacancies O_(2)^(-) species

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Molecular investigation into the transformation of recalcitrant dissolved organic sulfur in refinery sour water during stripping process

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Petroleum Science 2024年第3期21卷 2112-2119页

作者： Yu-Guo Li Chen He Chun-Mao Chen Fan Liu Quan Shi state key laboratory of heavy oil processing China University of Petroleum state key laboratory of Coal Mining and Clean Utilization Petrochina Ningxia Petrochemical Company

Refinery sour water primarily originates from the tops of towers in various units and coker condensate,and cannot be discharged directly to a wastewater treatment plant due to high levels of chemical oxygen demand(COD) and organic sulfur contents. Even after the recovery of H2S from the sour water by the stripping process, the effluent still contains a high concentration of dissolved organic sulfur(DOS), which can have a huge bad influence. While chemical composition of dissolved organic matter(DOM) in refinery wastewater has been extensively studied, the investigation of recalcitrant DOS from sour waters remains unclear. In the present study, chemical composition of sour water DOMs(especially DOS) was investigated using fluorescence spectroscopy(excitation-emission matrix, EEM) and mass spectrometry,including gas chromatography-mass spectrometry(GC-MS) and high-resolution Orbitrap MS. The GC-MS and EEM results showed that volatile and low-aromaticity compounds were effectively removed during the stripping process, while compounds with high hydrophilicity and humification degree were found to be more recalcitrant. The Orbitrap MS results showed that weak-polar oxygenated sulfur compounds were easier to be removed than oxygenated compounds. However, the effluent still contained significant amounts of sulfur-containing compounds with multiple sulfur atoms, particularly in the form of highly unsaturated and aromatic compounds. The Orbitrap MS/MS results of CHOS-containing compounds from the effluent indicate that the sulfur atoms may exist as sulfonates, disulfide bonds, thioethers. Understanding the composition and structure of sour water DOS is crucial for the development of effective treatment processes that can target polysulfide compounds and minimize their impact on the environment.

关键词： Molecular transformation Dissolved organic sulfur Stripping process Refinery sour water Orbitrap MS

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Hydrodynamics and OCM reaction performance in a bubbling fluidized bed reactor and a riser reactor

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Particuology 2024年第3期86卷 188-204页

作者： Min Cai Shuangzhu Kong Sheng Chen Mengxi Liu Chunxi Lu state key laboratory of heavy oil processing China University of PetroleumBeijing102249China china Special Equipment Inspection and Research Institute Beijing102249China

The reasonable reactor design is of great importance for increasing the C_(2) yield(C2H4 and C2H6)of the oxidative coupling of methane(OCM),and the OCM reactor should remove the heat released in reactions quickly and efficiently and minimize the consecutive reaction of ethylene to carbon oxides.The fluidized bed reactor is characterized by excellent heat transfer,superior mass transport,and large handling capacity,while fewer studies focused on large-scale fluidized bed reactors for the OCM reaction.Therefore,large cold-model experiments and computational fluid dynamics simulations were conducted to investigate hydrodynamics and the OCM reaction performance in a large-scale bubbling fluidized bed(BFB)and a large-scale riser.In the BFB reactor,consecutive reactions of ethylene are acute because of the strong gas back-mixing,high solids holdup,and non-uniform solids distribution.While the consecutive reactions of ethylene are negligible due to the plug flow structure and low solids holdup in the riser reactor.Further,both reactors can achieve isothermal operation for the OCM process.The C_(2) selectivity of 45.4% and C_(2) yield of 21.1% are obtained in the riser reactor,increasing by 20.3% and 5.8% individually than that in the BFB reactor.This study provides useful information and reference to the OCM reactor designandcommercialization.

关键词： Oxidative coupling of methane Bubbling fluidized bed reactor Riser reactor Hydrodynamics Isothermal operation

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Self-adaptive gas flow and phase change behaviors during hydrate exploitation by alternate injection of N2 and CO2

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Petroleum Science 2024年第3期21卷 2120-2129页

作者： Bo-Jian Cao Yi-Fei Sun Hong-Nan Chen Jin-Rong Zhong Ming-Long Wang Ming Wang Chang-Yu Sun Guang-Jin Chen state key laboratory of heavy oil processing China University of Petroleum School of Chemistry and Chemical Engineering Changsha University of Science & Technology

Since hydrate resources play a part of the stratigraphic framework structure in sediments,establishing a safe and economic method for hydrates exploitation remains the primary challenge to this day.Among the proposed methods,the spontaneous displacement of CH4from hydrate cages by CO2seems to be a perfect mechanism to address gas production and CO2storage,especially in today's strong demand for carbon reduction and replacing clean energy.After extensive lab researches,in the past decade,injecting a mixture of CO2and small molecule gas has become a key means to enhance displacement efficiency and has great potential for application.However,there is a lack of in-depth research on gas flow in the reservoir,while the injected gas always passes through low-saturated hydrate areas with high permeability and then occurs gas channel in a short term,finally resulting in the decreases in gas production efficiency and produced gas quality.Therefore,we explored a new injection-production mode of alternate injection of N2and CO2in order to fully coordinate the advantages of N2in enhanced hydrate decomposition and CO2in solid storage and heat compensation.These alternate "taking" and "storing" processes perfectly repair the problem of the gas channel,achieving self-regulation effect of CH4recovery and CO2storage.The 3-D experimental results show that compared to the mixed gas injection,CH4recovery is increased by>50% and CO2storage is increased by>70%.Additionally,this alternate injection mode presented a better performance in CH4concentration of produced gas and showed outstanding N2utilization efficiency.Further,we analyzed its self-adaptive gas flow mechanism and proposed an application model of "one injection and multiple production".We look forward to this study accelerating the application of CO2-CH4replacement technology.

关键词： Hydrate Replacement CH 4 recovery CO 2 storage Reservoir remediation

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Sensitive measurement of silver ions in environmental water samples integrating magnetic ion-imprinted solid phase extraction and carbon dot fluorescent sensor

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Chinese Chemical Letters 2024年第5期35卷 272-276页

作者： Shuangying Li Qingxiang Zhou Zhi Li Menghua Liu Yanhui Li state key laboratory of heavy oil processing College of Chemical Engineering and EnvironmentChina University of Petroleum-BeijingBeijing 102249China

Increasing use of silver in various fields has caused Ag^(+)pollution in water environment,taking great threats to people’s health.As a consequence,establishing rapid and reliable methods for sensitive determination of Ag^(+)is of great significance.Fluorescent(FL)sensors based on carbon dots(CDs),an excellent carbonaceous nanomaterial with strong and stable fluorescence,have absorbed extensive attentions in analysis of pollutants due to its advantages of carbon sources being readily available,low cost,easy operation and fast response.Moreover,ion-imprinting is a better way to increase the selectivity of the proposed method.Present work described an effective method for the sensitive measurement of silver ion in water samples in combination with magnetic ion-imprinted solid phase extraction and CDs based fluorescent sensor,which took full advantages of easy separation and high enrichment of magnetic solid phase extraction,high selectivity of ion-imprinting technology,and sensitivity and rapid response of fluorescent sensor from CDs.Sulfur-doped CDs derived from dithizone and magnetic ion-imprinted nanomaterial were prepared,and characterized with Fourier transform infrared spectroscopy and transmission electron microscope,etc.Magnetic Ag^(+)imprinted nanomaterial based solid phase extraction was employed for separating and enriching Ag^(+)from water samples.The significant parameters were optimized in detail.Under the optimal conditions,the proposed method provided good linearity in the range of 0.01-0.4μmol/L and low detection limit of 3 nmol/L.The reliability of the proposed method was validated with real water samples,and the results demonstrated that the proposed method was simple,robust,selective and sensitive detection tool for Ag^(+)in real water samples.

关键词： Carbon dots Ag^(+) Magnetic ion-imprinting Magnetic solid phase extraction Fluorescent sensor

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