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中国石化双氧水法制环氧丙烷工业开发及关键科技问题

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石油炼制与化工 2024年第1期55卷 130-134页

作者：夏长久于佳元林民朱斌彭欣欣舒兴田中石化石油化工科学研究院有限公司石油化工分子转化与反应工程全国重点实验室北京100083

为克服现有环氧丙烷(PO)生产技术弊端,中国石化采用表面富硅空心钛硅分子筛为活性组元的催化剂,开发了新型双氧水法制备环氧丙烷(HPPO)成套技术,建成了国内首套100 kt a HPPO工业装置。催化剂以表面富硅多空心钛硅分子筛为活性组元,采... 详细信息

为克服现有环氧丙烷(PO)生产技术弊端,中国石化采用表面富硅空心钛硅分子筛为活性组元的催化剂,开发了新型双氧水法制备环氧丙烷(HPPO)成套技术,建成了国内首套100 kt a HPPO工业装置。催化剂以表面富硅多空心钛硅分子筛为活性组元,采用高效羟基偶联黏结剂,提高了活性组元含量和催化剂强度。开发了器内低温原位复活技术。以复合助剂调控双氧水与骨架钛形成“五元环”过渡态,大幅提升PO选择性。开发出PO低温分离、萃取蒸馏和化学脱杂耦合的产品分离精制技术,提升产品质量。将PO废水作为炼油厂催化裂化装置的终止剂,使有机物裂解成乙烯、丙烯等低碳烃。与国外先进技术相比:双氧水转化率高3.3%,PO选择性高3.6%;产品中杂质总醛含量低80%,水分低50%;产品纯度达99.99%,优级品率达到100%。

关键词：空心钛硅分子筛 HPPO 环氧丙烷环氧化

A novel synthetic method of porous and nanoflower-like Al_(2)O_(3)/MoS_(2)catalyst for reduction of SO_(2)to elemental sulfur

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Nano Research 2023年第5期16卷 6076-6084页

作者： Yiqian Yang jiayuan yu yu Chen Gang Wang Chunshan Li Erqiang Wang Zhijian Peng School of Engineering and Technology China University of GeosciencesBeijing 100083China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

MoS_(2)nanoflowers are favored for their potential in the production of elemental sulfur due to abundant surface area and good catalytic performance for reducing SO_(2).A novel synthetic strategy of porous Al_(2)O_(3)supported on the MoS_(2)with nanoflower structure was *** effects of preparation concentration,calcination atmosphere,Al_(2)O_(3)contents on the growth of catalysts with nanoflower structure were systematically studied via X-ray diffraction(XRD),scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),transmission electron microscopy(TEM),Fourier transform infrared(FTIR)spectroscopy,Brunauer–Emmett–Teller(BET).The surface area was increased to 295.502 m^(2)/g and the amount of Lewis acid on the surface of the Al_(2)O_(3)/MoS_(2)catalyst was increased by adjusting the ratio of Al/*** porous and nanoflower structures of Al_(2)O_(3)/MoS_(2)catalysts promoted the sulfur selectivity without inhibiting the catalytic performance of MoS_(2).The conversion of SO_(2)and the selectivity of sulfur were 100%and 92%after 100 h life evaluation.

关键词： porous catalyst nanoflower reduction of SO_(2) sulfur production hydrogen

Chromium phosphide nanoparticles embedded in porous nitrogen-/phosphorus-doped carbon as efficient electrocatalysts for a nitrogen reduction reaction

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Carbon Energy 2022年第2期4卷 237-245页

作者： jiayuan yu Bin Chang Wanqiang yu Xiao Li Dufu Wang Zhinian Xu Xiaoli Zhang Hong Liu Weijia Zhou Institute for Advanced Interdisciplinary Research(IAIR) Shandong Collaborative Innovation Center of Technology and Equipements for Biological Diagnosis and TherapyUniversity of JinanJinanChina Shandong Best Environmental Technology Co.Ltd. JinanChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhouChina State Key Laboratory of Crystal Materials Shandong UniversityJinanChina

The resource recovery of heavy metals from effluent has significant environmental implications and potential commercial *** phosphide nanoparticles embedded in a nitrogen-/phosphorus-doped porous carbon matrix(CrP/NPC)are synthesized via a consecutive Cr^(6+)leachate treatment and resource recovery *** testing shows that CrP/NPC shows excellent nitrogen reduction reaction(NRR)performance,which yields the highest NH_(3) production rate of 22.56μg h^(−1) mg^(−1)_(cat).and Faradaic efficiency(16.37%)at−0.5 V versus the reversible hydrogen electrode in a 0.05M Na_(2)SO_(4) aqueous solution,as well as robust catalytic *** isotopic experiments using ^(15)N^(2) as a nitrogen source confirm that the detected NH_(3) is derived from the NRR ***,density functional theory(DFT)calculations show that the electron deficiency environment of the Cr site can significantly reduce the barrier of the NRR process and promote the formation of intermediate species.

关键词： biosynthesis carbon-based materials chromium phosphide leachate treatment nitrogen reduction reaction resource recovery

Waste-yeast biomass as nitrogen/phosphorus sources and carbon template:Environment-friendly synthesis of N,P-Mo_(2)C nanoparticles on porous carbon matrix for efficient hydrogen evolution

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Chinese Chemical Letters 2022年第6期33卷 3231-3235页

作者： jiayuan yu Wanqiang yu Bin Chang Xiao Li Jin Jia Dufu Wang Zhinian Xu Xiaoli Zhang Hong Liu Weijia Zhou Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong Institute for Advanced Interdisciplinary Research(iAIR)University of JinanJi'nan 250022China Shandong Best Environmental Technology Co. Ltd.Ji'nan 250J01 China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China State Key Laboratory of Crystal Materials Shandong UniversityJi'nan 250100China

Tailor-made advanced electrocatalysts with high active and stable for hydrogen evolution reaction(HER)play a key role in the development of hydrogen ***,a N,P-co-doped molybdenum carbide confined in porous carbon matrix(N,P-Mo_(2)C/NPC)with a hierarchical structure is prepared by a resources recovery *** N,P-Mo_(2)C/NPC compound exhibits outstanding HER activity with a low overpotential of 84 mV to achieve 10 mA/cm^(2),and excellent stability in alkaline *** electrochemical measurements confirm that the enhanced HER activity of N,P-Mo_(2)C/NPC is ascribe to the synergy of N,P-codoped and porous carbon *** functional theory calculations further reveal that the electron density of active sites on Mo_(2)C can be regulated by the N/P doping,leading to optimal H adsorption *** this work,the proof-of-concept resource utilization,a microorganism derived molybdenum carbide electrocatalyst for HER is fabricated,which may inaugurate a new way for designing electrocatalysts by the utilization of solid waste.

关键词： Hydrogen evolution reaction Molybdenum carbide Non-metal doping Resource utilization Solid waste management

Single-atom catalyst application in distributed renewable energy conversion and storage

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SusMat 2023年第2期3卷 160-179页

作者： Xiao Li Wenxiu Xu yuhan Fang Riming Hu jiayuan yu Hong Liu Weijia Zhou Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringUniversity of JinanJinanChina School of Biological Science and Technology University of JinanJinanChina Institute for Smart Materials&Engineering University of JinanJinanChina State Key Laboratory of Crystal Materials Shandong UniversityJinanChina

In recent years,owing to the depletion of fossil energy and the aggravation of environmental pollution,the conversion and storage of distributed renewable energy(such as solar energy,wind energy,and tidal energy)based on electrochemical technology have attracted extensive *** processes with high efficiency and high selectivity play a key role in clean energy conversion and *** the nearly 100%atomic utilization rate and unique catalytic activity,single-atom catalysts(SACs)have been rapidly developed and widely used in the field of energy conversion and *** this review,we first introduce the characteristics of ***,we focus on the application of SACs in energy conversion,including water electrolysis reaction,nitrogen reduction reaction,nitrate reduction reaction,oxygen reduction reaction,and carbon dioxide reduction *** terms of energy storage,we focus on supercapacitors and Li–S ***,we enumerate some of the methods for the synthesis of SACs in high metal loading or large ***,the main challenges and opportunities for this emerging field in the future are discussed and prospected.

关键词： electrocatalytic energy conversion energy storage single-atom catalysts

Effects of plasma ghrelin, obestatin, and ghrelin/obestatin ratio on blood pressure circadian rhythms in patients with obstructive sleep apnea syndrome

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Chinese Medical Journal 2014年第5期127卷 850-855页

作者： Liu Weiying yue Hongmei Zhang Jiabin Pu jiayuan yu Qin Department of Respiratory Medicine First Hospital of Lanzhou University Lanzhou Gansu 730000 China

Background Obstructive sleep apnea syndrome （OSAS） is strongly associated with obesity and with cardiovascular *** and obestatin are two peptides from the same source but have opposite *** of them can affect feeding and regulate vascular *** aim of this study was to investigate the relationship between plasma ghrelin,obestatin,the ratio of ghrelin and obestatin （G/O） and sleep parameters and blood pressure circadian rhythms in patients with *** This study enrolled 95 newly diagnosed over-weight OSAS patients （OSAS group）,30 body mass index （BMI）-match non-OSAS adults （over-weight group） and 30 non-OSAS normal weight adults （control group）.Polysomnography （PSG） was performed in the OSAS group and over-weight *** pressure of all subjects was monitored by means of 24-hour ambulatory blood pressure *** concentration of plasma ghrelin and obestatin was detected by enzyme-linked immunosorbent assay （ELISA）.Results Plasma ghrelin levels in the OSAS group and over-weight group were significantly lower than that of the control group （P ＜0.05）.Plasma obestatin levels were lower in the over-weight group and OSAS group,but there was no significant difference among the three *** blood pressure in OSAS patients was higher,and there was a significant difference in all blood pressure parameters compared to the control group,and in the daytime average diastolic blood pressure （DBP）,nocturnal average systolic blood pressure （SBP） and DBP,DBP variability values as compared to over-weight ***,there were significantly more non-dipper patterns of blood pressure （including hypertension and normotension） in the OSAS group than in the other two groups （P ＜0.01）.Correlation analysis showed that ghrelin levels had a significant correlation with BMI and nocturnal average DBP but not with PSG *** contrast,the G/O ratio had a negative correlation with apnea-hypopnea index （AHI）（P ＜0.05）,as well as a strong pos

关键词： obstructive sleep apnea syndrome ghrelin obestatin ghrelin/obestatin ratio blood pressure circadian rhythms

Enhanced electrocatalytic activity of Co@N-doped carbon nanotubes by ultrasmall defect-rich TiO2 nanoparticles for hydrogen evolution reaction

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Nano Research 2017年第8期10卷 2599-2609页

作者： jiayuan yu Weijia Zhou Tanli Xiong Aili Wang Shaowei Chen Benli Chu School of Environment and Energy Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control South China University of Technology Guangzhou Higher Education Mega Center Guangzhou 510006 China School of Physics and Telecommunication Engineering South China Normal University Guangzhou Higher Education Mega Center Guangzhou 510006 China Department of Chemistry and Biochemistry University of California 1156 High Street Santa Cruz CA 95064 USA

Despite being technically possible, splitting water to generate hydrogen is practically unfeasible, mainly because of the lack of sustainable and efficient earth-abundant catalysts for the hydrogen-evolution reaction （HER）. Herein, we report a durable and highly active electrochemical HER catalyst based on defect-rich TiO2 nanoparticles loaded on Co nanoparticles@N-doped carbon nanotubes （D-TiOdCo@NCT） synthesized by electrostatic spinning and a subsequent calcining process. The ultrasmall TiO2 nanoparticles are 1.5-2 nm in size and have a defect-rich structure of oxygen vacancies. D-TiO2/Co@NCT exhibits excellent HER catalytic activity in an acidic electrolyte （0.5 M H2SO4）, with a low onset potential of -57.5 mV （1 mA·cm^-2）, a small Tafel slope of 73.5 mV·dec^-1, and extraordinary long-term durability. X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy, and theoretical calculations confirm that the Ti3. defect-rich structure can effectively regulate the catalytic activity for electrochemical water splitting.

关键词： ultrasmall nanoparticle TiO2 defect structure carbon nanotube hydrogen-evolution reaction

Linking coral fluorescence phenotypes to thermal bleaching in the reef-building Galaxea fascicularis from the northern South China Sea

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Marine Life Science & Technology 2024年第1期6卷 155-167页

作者： Sanqiang Gong jiayuan Liang Gang Li Lijia Xu Yehui Tan Xinqing Zheng Xuejie Jin Kefu yu Xiaomin Xia Key Laboratory of Tropical Marine Bio-Resources and Ecology&Guangdong Provincial Key Laboratory of Applied Marine Biology South China Sea Institute of OceanologyChinese Academy of SciencesGuangzhou 510301China Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou) Guangzhou 510301China Coral Reef Research Center of China Guangxi UniversityNanning 53004China South China Institute of Environmental Sciences The Ministry of Ecology and Environment of PRCGuangzhou 510530China Third Institute of Oceanography Ministry of Natural ResourcesXiamen 361005China

Coral fluorescence phenotypes have been suggested as an adaptation to a broad range of environmental conditions,yet the mechanisms linking thermal bleaching tolerance in reef-building coral populations,associated with fluorescence phenotypes due to GFP-like proteins,remains *** this study,the relationship between the thermal sensitivity and phenotypic plasticity of corals was investigated using two phenotypes of Galaxea fascicularis,green and *** results reveal that brown *** was more susceptible to bleaching than green *** when exposed to a higher growth temperature of 32℃.Both phenotypes of *** were associated with the thermotolerant Symbiodiniaceae symbiont,Durusdinium ***,the brown *** showed a significant decrease in Symbiodiniaceae cell density and a significant increase in pathogenic bacteria abundance when the growth temperature was raised from 29 to 32℃.The physiological traits and transcriptomic profiles of Symbiodiniaceae were not notably affected,but there were differences in the transcriptional levels of certain genes between the two phenotype hosts of *** heat stress of 32℃,the gene encoding green fluorescent protein(GFP)-like and chromosome-associated proteins,as well as genes related to oxidative phosphorylation,cell growth and death showed lower transcriptional levels in the brown *** compared to the green ***,the results demonstrate that the green form of *** is better able to tolerate ocean warming and defend against pathogenic bacteria,likely due to higher gene transcription levels and defense ability.

关键词： Fluorescence phenotype Thermal bleaching Microbiome Galaxea fascicularis Ocean warming

Thyroid-stimulating hormone-thyroid hormone signaling contributes to circadian regulation through repressing clock2/npas2 in zebrafish

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Journal of Genetics and Genomics 2024年第1期51卷 61-74页

作者： Cheng Ji yue Ou Wangjianfei yu Jiaxin Lv Fanmiao Zhang Huashan Li Zeyun Gu jiayuan Li Zhaomin Zhong Han Wang Center for Circadian Clocks Soochow UniversitySuzhouJiangsu 215123China School of Biology and Basic Medical Sciences Suzhou Medical CollegeSoochow UniversitySuzhouJiangsu 215123China

Thyroid-stimulating hormone(TSH)is important for the thyroid gland,development,growth,and *** in TSH production or the thyrotrope cells within the pituitary gland cause congenital hypothyroidism(CH),resulting in growth retardation and neurocognitive *** human TSH is known to display rhythmicity,the molecular mechanisms underlying the circadian regulation of TSH and the effects of TSH-thyroid hormone(TH)signaling on the circadian clock remain *** we show that TSH,thyroxine(T4),triiodothyronine(T3),and tshba display rhythmicity in both larval and adult zebrafish and tshba is regulated directly by the circadian clock via both E′-box and *** tshba^(−/−)mutants manifest congenital hypothyroidism,with the characteristics of low levels of T_(4)and T_(3)and growth *** or overexpression of tshba alters the rhythmicity of locomotor activities and expression of core circadian clock genes and hypothalamic-pituitary-thyroid(HPT)axis-related ***,TSH-TH signaling regulates clock2/npas2 via the thyroid response element(TRE)in its promoter,and transcriptome analysis reveals extensive functions of Tshba in ***,our results demonstrate that zebrafish tshba is a direct target of the circadian clock and in turn plays critical roles in circadian regulation along with other functions.

关键词： Thyroid-stimulating hormone subunitβa (tshba) Thyroid hormone Circadian rhythm TALEN Zebrafish