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Eliminating H_(2)O/HF and regulating interphase with bifunctional tolylene-2,4-diisocyanate(TDI)additive for long life Li-ion battery 被引量:1
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作者 Xueyi Zeng Xiang Gao +8 位作者 Peiqi Zhou Haijia Li Xin He Weizhen Fan Chaojun Fan Tianxiang Yang Zhen Ma Xiaoyang Zhao Junmin Nan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期519-528,I0011,共11页
Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challengi... Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challenging.Especially when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the interphase.In order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated temperature.After 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 C.In contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated temperatures.The analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense interphase.The existence of this interphase is thought to substantially enhance the cycling performance of the LIBs.This work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development. 展开更多
关键词 Graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)battery Tolylene-2 4-diisocyanate Long-cycling performance H_(2)O/HF eliminated additive
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A cascade of in situ conversion of bicarbonate to CO_(2) and CO_(2) electroreduction in a flow cell with a Ni-N-S catalyst
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作者 Linghui Kong Min Wang +6 位作者 Yongxiao Tuo Shanshan Zhou Jinxiu Wang Guangbo Liu Xuejing Cui Jiali Wang Luhua Jiang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期183-193,I0005,共12页
Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electroche... Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals. 展开更多
关键词 S doped Ni-N-C single atom catalysts CO_(2)electrochemical reduction DFT calculations Membrane electrode assembly Reduction of bicarbonate
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水泥石防CO_2、H_2S腐蚀性能的室内研究 被引量:13
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作者 万伟 陈大钧 《钻井液与完井液》 CAS 2009年第5期57-59,共3页
通过分析CO_2、H_2S对水泥石的腐蚀机理,采用一种新型的通过聚合反应生成的线性水溶性高分子乳状液防腐蚀剂,考察了在腐蚀条件下,净水泥浆、加入新型防腐蚀剂的水泥浆、加入填充材料的水泥浆以及加入防腐蚀剂和填充材料以后的水泥浆形... 通过分析CO_2、H_2S对水泥石的腐蚀机理,采用一种新型的通过聚合反应生成的线性水溶性高分子乳状液防腐蚀剂,考察了在腐蚀条件下,净水泥浆、加入新型防腐蚀剂的水泥浆、加入填充材料的水泥浆以及加入防腐蚀剂和填充材料以后的水泥浆形成的水泥试块的抗压强度、渗透率和外貌形态变化,同时通过XL-30型扫描电子显微镜对水泥试块的内部结构进行了观察。实验表明,在水泥浆中同时加入新型防腐蚀剂和填充材料以后,水泥石的防腐蚀能力得到极大的提高,相对净浆来说,水泥石渗透率降低率达80.7%;由于防腐蚀剂具有一定的缓凝作用,所以水泥石抗压强度会受到一定的影响,若有需要,建议通过加大促凝剂量来调节其抗压强度值。 展开更多
关键词 水泥石 防腐蚀剂 CO_2腐蚀 H_2S腐蚀 腐蚀机理
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在含CO_2/H_2S介质中油气田用钢的腐蚀研究进展 被引量:14
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作者 赵永峰 王吉连 +1 位作者 左禹 熊金平 《石油化工腐蚀与防护》 CAS 2010年第1期1-8,共8页
研究了CO_2和H_2S对油气田开发用钢材的腐蚀机理、分析了影响因素以及防护措施,并对研究进展情况进行综述。指出目前国内各油气田关于CO_2/H_2S的腐蚀问题,一方面对腐蚀机理的认识还不够全面与深入,另一方面其防护技术研究尚未达到系统... 研究了CO_2和H_2S对油气田开发用钢材的腐蚀机理、分析了影响因素以及防护措施,并对研究进展情况进行综述。指出目前国内各油气田关于CO_2/H_2S的腐蚀问题,一方面对腐蚀机理的认识还不够全面与深入,另一方面其防护技术研究尚未达到系统化和实用化的程度。 展开更多
关键词 钢材 CO_2/H_2S腐蚀 腐蚀因素 防护措施
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含CO_2-H_2S酸性气田冲刷腐蚀概述 被引量:3
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作者 周霄骋 刘智勇 邢云颖 《中国特种设备安全》 2016年第8期1-5,共5页
天然气管线的安全服役对国民生产和生活意义重大。近年来,随着对含高浓度CO_2、H_2S等强腐蚀性介质酸性气田的大量开发,输送压力和流速不断提高,通过采用传统脱硫、脱CO_2、缓蚀剂等技术在实际应用中效果有限,导致天然气管线的腐蚀失效... 天然气管线的安全服役对国民生产和生活意义重大。近年来,随着对含高浓度CO_2、H_2S等强腐蚀性介质酸性气田的大量开发,输送压力和流速不断提高,通过采用传统脱硫、脱CO_2、缓蚀剂等技术在实际应用中效果有限,导致天然气管线的腐蚀失效情况仍比较严重,尤其是三通、法兰、焊缝等特殊位置。本文通过阐述CO_2-H_2S酸性气田冲刷腐蚀的特征和影响因素,总结了含CO_2-H_2S酸性气田中冲刷腐蚀的研究进展,指出研究天然气高速冲刷与薄液电化学相互作用和腐蚀发生机理对预防天然气管线钢的冲刷腐蚀有较重要的意义。 展开更多
关键词 CO_2 H_2S 冲刷 薄液膜 酸性气田
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Simultaneous Removal of COS and H_2S at Low Temperatures over Nanoparticle a-FeOOH Based Catalysts 被引量:1
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作者 Zhihua Gao, Chunhu Li, Kechang XieState Key Lab of C1 Chemistry and Technology, Institute of Coal Chemical Engineering, Taiyuan University of Technology,Taiyuan 030024, China 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2003年第1期37-42,共6页
Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^... Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^(-1), while the removal performance of H_2S withcatalysts was investigated using the thermal gravimetric method. The results show that the catalystsare highly active for COS hydrolysis at low temperatures (≤60 ℃) and high gas hourly spacevelocity, and the highest activity can reach 100%. The catalyst is particularly stable for 12 h, andno deactivation is observed. Nanoparticle α-FeOOH prepared using hydrated iron sulfate showshigher COS hydrolysis activity, and the optimum calcination temperature for the catalyst is 260 ℃.In addition, the catalysts can remove COS and H_2S simultaneously, and 60 ℃ is favorable for theremoval of H_2S. The compensation effect exists in nanoparticle-based catalysts. 展开更多
关键词 nanoparticle α-FeOOH COS hydrolysis removal of H_2S compensationeffect
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Switching CO_(2) Electroreduction Selectivity Between C_(1) and C_(2) Hydrocarbons on Cu Gas-Diffusion Electrodes 被引量:1
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作者 Jianfang Zhang Zhengyuan Li +6 位作者 Rui Cai Tianyu Zhang Shize Yang Lu Ma Yan Wang Yucheng Wu Jingjie Wu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第2期17-25,共9页
Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important r... Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness,local pH,and facet in governing the selectivity toward C_(1)or C_(2)hydrocarbons.The selectivity toward C_(2)H_(4) progressively increases,while CH_(4) decreases steadily upon lowering the Cu oxidation species fraction.At a relatively low electrodeposition voltage of 1.5 V,the Cu gas-diffusion electrode with the highest Cu^(δ+)/Cu^(0)ratio favors the pathways of∗CO hydrogenation to form CH_(4) with maximum Faradaic efficiency of 65.4%and partial current density of 228 mA cm^(−2)at−0.83 V vs RHE.At 2.0 V,the Cu gas-diffusion electrode with the lowest Cu^(δ+)/Cu^(0)ratio prefers C-C coupling to form C_(2)+products with Faradaic efficiency topping 80.1%at−0.75 V vs RHE,where the Faradaic efficiency of C_(2)H_(4) accounts for 46.4%and the partial current density of C_(2)H_(4) achieves 279 mA cm^(−2).This work demonstrates that the selectivity from CH_(4) to C_(2)H_(4) is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes. 展开更多
关键词 C_(2)H_(4) CH_(4) CO_(2)electroreduction ELECTRODEPOSITION switchable selectivity
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基于CSE/H_2S体系探讨葱白提取物对H_2S催化酶及趋化因子CX3CL1的作用机制
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作者 雷杰 郑琼莉 段刚峰 《新疆医科大学学报》 CAS 2023年第11期1444-1449,共6页
目的研究葱白提取物对动脉粥样硬化(AS)大鼠CX3C趋化因子配体1(CX3CL1)、CX3C趋化因子受体1(CX3CR1)、胱硫醚β合成酶(CBS)、3-巯基丙酮酸硫基转移酶(3MST)表达的影响及相互作用机制。方法纯种健康雄性SD大鼠,SPF级,体重(200±20)g,... 目的研究葱白提取物对动脉粥样硬化(AS)大鼠CX3C趋化因子配体1(CX3CL1)、CX3C趋化因子受体1(CX3CR1)、胱硫醚β合成酶(CBS)、3-巯基丙酮酸硫基转移酶(3MST)表达的影响及相互作用机制。方法纯种健康雄性SD大鼠,SPF级,体重(200±20)g,共40只,随机选择10只作为正常组,另外30只制备大鼠AS模型,再随机分为模型组、葱白提取物组、辛伐他汀组,每组各10只。正常组以基础饲料喂养,模型组、葱白提取物组、辛伐他汀组均以高脂维生素D3饲料喂养。从第5周开始,葱白提取物组大鼠给予配置好的葱白提取物溶液10 mL/kg体质量灌胃,辛伐他汀组大鼠给予辛伐他汀混悬液10 mL/kg体质量灌胃;正常组和模型组均给予等容积生理盐水10 mL/kg体质量灌胃,共连续8周。在第12周时,留取大鼠血液,分离主动脉。采用生化检测、HE染色、Western blot、RT-PCR检测脂质代谢、H_(2)S催化酶、趋化因子及基质金属蛋白酶表达。结果与模型组比较,葱白提取物组及辛伐他汀组大鼠血清总胆固醇、甘油三酯、低密度脂蛋白胆固醇、载脂蛋白B浓度均降低(P<0.05),高密度脂蛋白胆固醇浓度升高(P<0.05)。与模型组比较,葱白提取物组及辛伐他汀组斑块内部的胆固醇结晶较少,管腔狭窄程度较轻。与模型组比较,葱白提取物组和辛伐他汀组CX3CL1 mRNA、CX3CR1 mRNA、MMP7 mRNA、MMP9 mRNA表达均下调。与模型组比较,葱白提取物组和辛伐他汀组大鼠主动脉组织中3MST、CBS蛋白相对表达量升高(P<0.05),而CX3CL1、CX3CR1蛋白相对表达量降低(P<0.05)。结论葱白提取物可通过调控内源性H_(2)S生成体系,抑制CX3CL1、CX3CR1表达、降低MMP7、MMP9活性,发挥抗动脉粥样硬化作用。 展开更多
关键词 葱白提取物 动脉粥样硬化 胸痹 CX3CL1/CX3CR1 H_(2)S
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Effect of carbon dioxide on oxy-fuel combustion of hydrogen sulfide:An experimental and kinetic modeling
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作者 Xun Tao Fan Zhou +6 位作者 Xinlei Yu Songling Guo Yunfei Gao Lu Ding Guangsuo Yu Zhenghua Dai Fuchen Wang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第7期105-117,共13页
CO_(2) is an important component in the acid gas and it is necessary to study the effect of CO_(2) presence on the oxy-fuel combustion of H_(2)S with particular focus on the formation of carbonyl sulfide(COS).The oxyf... CO_(2) is an important component in the acid gas and it is necessary to study the effect of CO_(2) presence on the oxy-fuel combustion of H_(2)S with particular focus on the formation of carbonyl sulfide(COS).The oxyfuel combustion of acid gas was conducted in a coaxial jet double channel burner.The distribution of flame temperature and products under stoichiometric condition along axial(R=0.0)and radial at about 3.0 mm(R=0.75)were analyzed,respectively.The Chemkin-Pro software was used to analyze the rate of production(ROP)for gas products and the reaction pathway of acid gas combustion.Both experimental and simulation results showed that acid gas combustion experienced the H2S chemical decomposition,H_(2)S oxidation and accompanied by H_(2) oxidation.The CO_(2) presence reduced the peak flame temperature and triggered the formation of COS in the flame area.COS formation at R=0.0 was mainly through the reaction of CO_(2) and CO with sulfur species,whereas at R=0.75 it was through the reaction of CO with sulfur species.The ROP results indicated that H_(2) was mainly from H_(2)O decomposition in the H_(2)S oxidation stage,and COS was formed by the reaction of CO_(2) with H_(2)S.ROP and other detailed analysis further revealed the role of H,OH and SH radicals in each stage of H_(2)S conversion.This study revealed the COS formation mechanisms with CO_(2) presence in the oxy-fuel combustion of H_(2)S and could offer important insights for pollutant control. 展开更多
关键词 Carbon dioxide Oxy-fuel combustion of H_(2)S Reaction pathway KINETICS OXIDATION
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Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO_(2)adsorbents
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作者 Chao Yang Zhelin Su +3 位作者 Yeshuang Wang Huiling Fan Meisheng Liang Zhaohui Chen 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第4期233-241,共9页
A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as precursors.The effect of gel drying temperature on the structure and desulfurizati... A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as precursors.The effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in detail.It is found that the low drying temperature led to a weak interaction among EG,Si AOH/H_(2)O and the nitrates in the gel system,which caused the oxidation of EG by NO3-and formed zinc glyoxylate complex during the gel calcination process,whereas this oxidation process also occurred at a high drying temperature during the gel drying process.The formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of Zn O,which resulted in the inferior desulfurization performance of adsorbents despite they have smaller Zn O nanoparticles.The gel dried at 120°C formed the hydrogen bonds between EG and Si AOH/H_(2)O and a strong interaction between zinc oxo-clusters and NO3-was also found in the gel system,which avoided the oxidation of EG by NO3-during the preparation process and the Zn O nanoparticles with sizes of 6 nm were formed by a combustion method.The adsorbent affords a highest sulfur capacity of 104.9 mg·g^(-1) in this case.In addition,the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area. 展开更多
关键词 Sol-gel method Drying temperature H_(2)S removal Zinc-silica composites Hydrogen bonds
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Regulation of excitation energy transfer in Sb-alloyed Cs_(4)MnBi_(2)Cl_(12) perovskites for efficient CO_(2) photoreduction to CO and water oxidation toward H_(2)O_(2)
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作者 Haiwen Wei Zhen Li +7 位作者 Honglei Wang Yang Yang Pengfei Cheng Peigeng Han Ruiling Zhang Feng Liu Panwang Zhou Keli Han 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第7期18-24,I0001,共8页
Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,... Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer. 展开更多
关键词 Pb-free perovskites Energy band modulation Perovskite photocatalysis photocatalytic CO_(2)reduction Water oxidation to H_(2)O_(2)
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S型异质结光催化剂ZnFe_(2)O_(4)/WO_(3)的构筑及光催化还原CO_(2)性能 被引量:1
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作者 刘平 朱成才 +1 位作者 李艳阳 要红昌 《无机化学学报》 SCIE CSCD 北大核心 2024年第1期197-208,共12页
通过在WO_(3)纳米片表面负载ZnFe_(2)O_(4)纳米颗粒,构建了一系列S型异质结光催化剂ZnFe_(2)O_(4)/WO_(3),并研究了其光催化CO_(2)还原性能。在没有助催化剂和牺牲剂的条件下,所制备的ZnFe_(2)O_(4)/WO_(3)复合材料可对CO_(2)与水蒸汽... 通过在WO_(3)纳米片表面负载ZnFe_(2)O_(4)纳米颗粒,构建了一系列S型异质结光催化剂ZnFe_(2)O_(4)/WO_(3),并研究了其光催化CO_(2)还原性能。在没有助催化剂和牺牲剂的条件下,所制备的ZnFe_(2)O_(4)/WO_(3)复合材料可对CO_(2)与水蒸汽进行光催化反应。优化后的材料光照5 h后CO_(2)还原产物CO和CH_(4)的产量分别为7.87和4.88μmol·g^(-1)。相对于单相组分,CO和CH_(4)的产量明显提高。光催化活性的提高,归因于ZnFe_(2)O_(4)和WO_(3)异质结的形成以及光生载流子的S型电荷传输模式。 展开更多
关键词 CO_(2)还原 光催化活性 ZnFe_(2)O_(4)/WO_(3) 异质结 S型电荷传输模式
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Synergetic enhancement of selectivity for electroreduction of CO_(2)to C_(2)H_(4)by crystal facet engineering and tandem catalysis over silver-incorporated-cuprous oxides
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作者 Gang Dong Chuang Xue +3 位作者 Meng Li Tiantian Zhang Dongsheng Geng Li-Min Liu 《Materials Reports(Energy)》 2023年第2期164-172,I0004,共10页
Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electr... Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts. 展开更多
关键词 Cu_(2)O/Ag tandem catalysts Facet-dependent selectivity CO_(2)reduction reaction C_(2)H_(4) ELECTROCATALYSIS Synergistic effect
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宽负荷下切圆燃煤锅炉H_(2)S分布特性的数值模拟 被引量:1
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作者 邓磊 袁茂博 +3 位作者 杨家辉 韩磊 姜家豪 车得福 《煤炭学报》 EI CAS CSCD 北大核心 2024年第6期2887-2895,共9页
锅炉采用空气分级燃烧降低NO_(x)排放的同时也提高了主燃区H_(2)S体积分数。炉墙壁面过高的H_(2)S体积分数是加剧水冷壁高温腐蚀的重要因素。为保障新能源并网发电,大型燃煤机组灵活调峰的需求增加,不同负荷下的水冷壁近壁面H_(2)S分布... 锅炉采用空气分级燃烧降低NO_(x)排放的同时也提高了主燃区H_(2)S体积分数。炉墙壁面过高的H_(2)S体积分数是加剧水冷壁高温腐蚀的重要因素。为保障新能源并网发电,大型燃煤机组灵活调峰的需求增加,不同负荷下的水冷壁近壁面H_(2)S分布特性值得关注。通过正交试验分析了切圆燃煤锅炉运行参数对水冷壁近壁面H_(2)S体积分数分布的影响。选取一台超临界600 MW切圆燃煤锅炉建立数值模型,设计L_(16)(4^(5))正交工况,覆盖100%BMCR、75%THA,50%THA以及35%BMCR四种负荷。建立了自定义SO_(x)生成模型以确定燃料硫的析出和转化路径,模型包含多表面反应子模型以描述焦炭与O_(2)/CO_(2)/H_(2)O等3种气体的异相反应,并确定焦炭气化反应消耗量占总消耗量的比例,进而对炉膛H_(2)S空间分布进行了模拟计算。研究表明,近壁面高体积分数H_(2)S区域主要位于投运燃烧器层中最下层燃烧器以下以及最上层燃烧器以上至SOFA层之间,烟气切圆沿炉膛高度增加逐渐增大是造成后一区域H_(2)S体积分数较高的重要原因。35%BMCR负荷下水冷壁重点区域的H_(2)S平均体积分数为364μL/L,明显低于其他负荷。锅炉运行参数对重点区域H_(2)S体积分数影响程度的排序为:锅炉负荷>一次风率>主燃区空气过量系数>假想切圆直径>燃烧器竖直摆角。 展开更多
关键词 切圆燃煤锅炉 宽负荷 H2S分布 正交分析 数值模拟
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环境因素对BT80S-5Cr抗CO_(2)/H_(2)S腐蚀套管均匀腐蚀速率的影响
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作者 石晓霞 雷鸣 +2 位作者 詹飞 强强 张程远 《钢管》 CAS 2024年第5期15-19,共5页
通过模拟国内某油田腐蚀工况,采用高温高压釜模拟腐蚀试验,利用失重法研究试验周期、温度、CO_(2)及H2S分压环境因素对BT80S-5Cr油套管均匀腐蚀速率的影响。研究表明,随着试验周期的延长,试验钢均匀腐蚀速率逐渐降低,且降幅趋于平缓,试... 通过模拟国内某油田腐蚀工况,采用高温高压釜模拟腐蚀试验,利用失重法研究试验周期、温度、CO_(2)及H2S分压环境因素对BT80S-5Cr油套管均匀腐蚀速率的影响。研究表明,随着试验周期的延长,试验钢均匀腐蚀速率逐渐降低,且降幅趋于平缓,试验周期360 h是BT80S-5Cr在该油气田模拟工况下衡量耐蚀性能的最佳试验周期;随着试验温度的提高,试验钢均匀腐蚀速率逐渐增加,试验温度100℃的试验钢的均匀腐蚀速率是试验温度40℃时的均匀腐蚀速率的1.67倍;随着CO_(2)分压的提高,试验钢均匀腐蚀速率逐渐增加,CO_(2)分压1.0 MPa的试验钢均匀腐蚀速率是不含CO_(2)时的均匀腐蚀速率的10倍;随着H2S分压的提高,试验钢均匀腐蚀速率逐渐降低,微量H_(2)S气体的引入对试验钢电化学腐蚀行为有一定的抑制作用。 展开更多
关键词 套管 BT80S-5Cr 腐蚀速率 CO_(2)/H_(2)S
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湿气环境中CO_(2)-H_(2)S在α-Fe(110)密排面上吸附与点蚀机理研究
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作者 李金灵 马文骏 +2 位作者 朱世东 屈撑囤 付安庆 《表面技术》 EI CAS CSCD 北大核心 2024年第20期82-93,共12页
目的从微观尺度探究CO_(2)-H_(2)S(CO_(2)和H_(2)S共存)在湿气管道顶部的吸附特性,进而揭示点蚀机理。方法基于密度泛函理论的第一性原理,利用Materials Studio构建CO_(2)、H_(2)S和CO_(2)-H_(2)S在α-Fe(110)密排面的吸附模型,对CO_(2)... 目的从微观尺度探究CO_(2)-H_(2)S(CO_(2)和H_(2)S共存)在湿气管道顶部的吸附特性,进而揭示点蚀机理。方法基于密度泛函理论的第一性原理,利用Materials Studio构建CO_(2)、H_(2)S和CO_(2)-H_(2)S在α-Fe(110)密排面的吸附模型,对CO_(2)、H_(2)S和CO_(2)-H_(2)S在α-Fe(110)面的吸附能、局域态密度、分波态密度和差分电荷密度进行仿真;利用高温高压釜模拟CO_(2)-H_(2)S-Cl^(-)腐蚀环境,分析L360钢在湿气环境中的腐蚀行为;最后,揭示含Cl^(-)湿气管道顶部CO_(2)-H_(2)S吸附机制与点蚀机理。结果CO_(2)、H_(2)S、CO_(2)-H_(2)S及CO_(2)-H_(2)S-Cl^(-)在最稳定位置时的吸附能分别为-4.065、-3.961、-8.538、-12.775e V,表明相较于CO_(2)与H_(2)S单独吸附,CO_(2)-H_(2)S在α-Fe(110)面的吸附能更负,Cl^(-)会进一步降低CO_(2)-H_(2)S的吸附能;且CO_(2)在与H_(2)S竞争环境电子中占优势;Cl^(-)会使CO_(2)-H_(2)S的局域态密度峰值降低,转移趋势为失去电子,基体和腐蚀介质的电子向着低能级跃迁释放出更多能量,进而加强了Fe与CO_(2)-H_(2)S间的化学键强度;Cl^(-)的2p轨道与Fe的3d轨道在-6.8 eV和-5.7 eV发生重叠,Cl^(-)被吸附到Fe表面并与Fe形成化学键生成氯化物,进而改变腐蚀产物膜的组分与结构,削弱产物膜的致密性和稳定性,减弱腐蚀阻抗力。在含Cl^(-)湿气的CO_(2)-H_(2)S环境中,液相中的Cl^(-)浓度升高,使L360钢的气相平均腐蚀速率逐渐增大,最高达2.935mm/a,点蚀越发严重。结论CO_(2)与H_(2)S在α-Fe(110)面吸附存在一定的协同和竞争作用,协同促进金属的腐蚀,FeCO3会优先沉积成膜,但H_(2)S会抑制FeCO3的生长,腐蚀产物以FeS为主;Cl^(-)会增强CO_(2)-H_(2)S与α-Fe(110)面间的作用力,弱化腐蚀产物膜层的保护性,进一步加速金属腐蚀、尤其是点蚀。 展开更多
关键词 CO_(2)-H_(2)S Cl^(-) 第一性原理 α-Fe(110)密排面 吸附特征 腐蚀机理
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衰竭底水气藏注CO_(2)提高天然气采收率与碳封存机理
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作者 张烈辉 熊伟 +5 位作者 赵玉龙 文绍牧 曹正林 刘莉莉 罗山贵 汪永朝 《天然气工业》 EI CAS CSCD 北大核心 2024年第4期25-38,I0001,共15页
气藏注CO_(2)提高天然气采收率并实现碳封存有望成为大幅度提高天然气产量与碳减排协同的潜在关键技术。为了给底水气藏注CO_(2)高效开发提供指导,针对地层水盐度对CO_(2)-CH_(4)-H_(2)O-NaCl体系相平衡影响、气藏注气过程中压力变化对C... 气藏注CO_(2)提高天然气采收率并实现碳封存有望成为大幅度提高天然气产量与碳减排协同的潜在关键技术。为了给底水气藏注CO_(2)高效开发提供指导,针对地层水盐度对CO_(2)-CH_(4)-H_(2)O-NaCl体系相平衡影响、气藏注气过程中压力变化对CO_(2)-CH_(4)-H_(2)O-NaCl体系相平衡影响、注采方案对注CO_(2)提高气藏采收率影响、盐度对注CO_(2)提产及封存影响等目前认识不清的问题开展了CO_(2)-CH_(4)-H_(2)O-NaCl体系相平衡规律及注CO_(2)提采与封存数值模拟研究。研究结果表明:①随着盐度增加,CO_(2)和CH_(4)在盐水中的溶解度降低,液相的密度和黏度增加,盐度对气相性质几乎没有影响;②随着压力增加,CO_(2)和CH_(4)在液相中的溶解度均增加,气相、液相密度和黏度均增加,液相偏差因子随压力增加而增加,气相偏差因子先减小后增加;③同注同采方案CH_(4)产量更稳定且产出的CO_(2)少,而先注后采方案则会加速CO_(2)与CH_(4)的混合,CO_(2)封存量低,前者更适合注CO_(2)提采及封存;④在不考虑盐析效应的前提下,盐度对CH_(4)采收率和CO_(2)封存量的影响几乎可以忽略不计,不同盐度的衰竭底水气藏中CH_(4)采收率均超过80%、CO_(2)封存率均超过99%,短期注CO_(2)过程中,CO_(2)主要以气态或超临界态的形式被封存,少部分CO_(2)溶解在液相中,100年后CO_(2)在液相中的溶解质量分数约为5%。结论认为,衰竭底水气藏注CO_(2)能增压补能、驱替置换残余天然气,提高采收率并实现碳封存。 展开更多
关键词 衰竭底水气藏 注二氧化碳 提高气藏采收率 碳封存 e-CPA状态方程 CO_(2)-CH_(4)-H_(2)O-Nacl体系 相态变化规律
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硫化氢气体在金属有机骨架中吸附机理的分子模拟研究
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作者 孟筠青 周子涵 +1 位作者 皮若楠 王婕 《安全与环境学报》 CAS CSCD 北大核心 2024年第1期99-107,共9页
研究硫化氢(H_(2)S)气体在金属有机骨架(Metal Organic Frameworks, MOFs)材料中的吸附机理,对应用MOFs材料控制城市地下有限空间内的H_(2)S气体具有重要意义。以不同类型的MOFs材料作为研究对象,基于Materials Studio软件建立了MOFs-H_... 研究硫化氢(H_(2)S)气体在金属有机骨架(Metal Organic Frameworks, MOFs)材料中的吸附机理,对应用MOFs材料控制城市地下有限空间内的H_(2)S气体具有重要意义。以不同类型的MOFs材料作为研究对象,基于Materials Studio软件建立了MOFs-H_(2)S吸附体系,应用巨正则蒙特卡洛(Rand Canonical Monte Carlo, GCMC)方法及分子动力学(Molecular Dynamics, MD)理论研究了相互作用能、吸附热、金属位点、官能团等的影响,在分子层面讨论了H_(2)S气体在MOFs中的吸附特性及机理。应用等温吸附试验验证了所使用分子模型及力场的可靠性。结果表明:不同金属位点对于吸附量有较大影响,对H_(2)S气体的吸附作用由强到弱依次为Mg^(2+)、Ni^(2+)、Co^(2+)、Mn^(2+)、Zn^(2+);亲水性官能团的引入利于H_(2)S气体的吸附捕捉;UiO-66-Cu因其团簇为网状结构更利于H_(2)S气体的捕捉与吸附。同时,该研究建立了吸附热方程,提供了MOFs吸附效果评判标准,为MOFs材料应用于城市地下有限空间吸附H_(2)S气体提供了理论依据。 展开更多
关键词 安全工程 金属有机骨架(MOFs)材料 H_(2)S气体吸附 分子模拟 有限空间
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复合微生物除臭液制备及其安全性与除臭效果评估
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作者 李春艳 崔志峰 +2 位作者 王景春 李春华 贺永明 《辽宁农业职业技术学院学报》 2024年第4期18-23,33,共7页
为制备复合微生物除臭液并评估其除臭效果和安全性,试验通过特殊营养液、光照厌氧处理从鸡粪样品中富集和扩增培养微生物菌液,从中筛选出最优复合微生物除臭液J9和J10,测定其生长曲线,并进行除臭效果试验和小鼠急性毒性检测。结果表明:J... 为制备复合微生物除臭液并评估其除臭效果和安全性,试验通过特殊营养液、光照厌氧处理从鸡粪样品中富集和扩增培养微生物菌液,从中筛选出最优复合微生物除臭液J9和J10,测定其生长曲线,并进行除臭效果试验和小鼠急性毒性检测。结果表明:J9和J10在扩增培养第2 d进入对数期,在第5~6 d进入稳定期。与不喷洒除臭液的对照组相比,筛选出的最优复合微生物除臭液J9和J10对鸡粪产生的NH_(3)和H_(2)S的去除率可高达82.41%和76.18%,显著(P<0.05)高于不喷洒除臭液的对照组。安全评价结果显示,复合微生物除臭液对小鼠急性经口毒性LD_(50)>40 g/kg体重,属于实际无毒级物质,具有较好的安全性。说明该复合微生物除臭液在实际应用中具有高效的除臭能力和安全性,并易制备。 展开更多
关键词 复合微生物除臭液 生长曲线 NH_(3) H_(2)S 急性毒性评价
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不同脱水剂和催化剂对油酸基咪唑啉缓蚀性能的影响
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作者 赵景茂 赵萃红 张存丽 《石油化工腐蚀与防护》 CAS 2024年第5期6-8,38,共4页
选用二甲苯、活性氧化铝和硼酸等作为脱水剂或催化剂,分别合成了三种油酸基咪唑啉,利用红外光谱对咪唑啉的结构进行了表征,使用质量损失法、极化曲线法和交流阻抗法等技术比较了三种油酸基咪唑啉缓蚀剂在H_(2)S/CO_(2)饱和的高矿化度溶... 选用二甲苯、活性氧化铝和硼酸等作为脱水剂或催化剂,分别合成了三种油酸基咪唑啉,利用红外光谱对咪唑啉的结构进行了表征,使用质量损失法、极化曲线法和交流阻抗法等技术比较了三种油酸基咪唑啉缓蚀剂在H_(2)S/CO_(2)饱和的高矿化度溶液中对碳钢的缓蚀性能。结果表明,使用活性氧化铝催化合成的咪唑啉缓蚀效果最好。 展开更多
关键词 H_(2)S/CO_(2)腐蚀 咪唑啉缓蚀剂 催化剂 脱水剂
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