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Highly efficient photo-thermal synergistic catalysis of CO_(2)methanation over La_(1-x)Ce_(x)NiO_(3)perovskite-catalyst

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Nano Research 2024年第9期17卷 7945-7956页

作者： Ting Li Zhen-yu Zhang De-Cun Luo Bo-yu Xu Rong-Jiang Zhang Ji-Long Yao Dan Li Tao Xie Institute of Industrial Catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

Solar-driven photo-thermal catalytic CO_(2)methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases ***,designing advanced photo-thermal catalysts remains a research challenge for CO_(2)methanation *** this work,a series of ABO3(A=lanthanide,B=transition metal)perovskite catalysts with Ce-substituted LaNiO3(La_(1-x)Ce_(x)NiO_(3),x=0,0.2,0.5,0.8,1)were synthesized for CO_(2)*** La_(0.2)Ce_(0.8)NiO_(3) exhibited the highest CH_(4) formation rate of 258.9 mmol·g^(-1)·hcat-1,CO_(2)conversion of 55.4%and 97.2%CH_(4) selectivity at 300℃with the light intensity of 2.9 W·cm^(-2).Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties *** partial substitution of the A-site provided more active sites for the adsorption and activation of CO_(2)/H_(2).The sources of the active sites were considered to be the oxygen vacancies(O_(v))created by lattice distortions due to different species of ions(La^(3+),Ce^(4+),Ce^(3+))and exsolved Ni0 by H_(2)*** catalysts have excellent light absorption absorbance and low electron-hole(e^(-)/h^(+))recombination rate,which greatly contribute to the excellent performance in photo-thermal synergistic catalysis(PTC)CO_(2)*** results of in situ irradiated electron paramagnetic resonance spectrometer(ISI-EPR)and ISI-X-ray photoelectron spectroscopy(XPS)indicated that the aggregation of unpaired electrons near the defects and Ni metal(from La and Ce ions to ov and Ni0)accelerated adsorption and activation of CO_(2)/H_(2).At last,the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)*** in situ precipitation of the B-site enhanced the dispersion of Ni,while its enriched photoelectrons upon illumination further promote hydrogen *** H^(*)spillover accelerated t

关键词： photo-thermal catalysis CO_(2)methanation perovskite A-site substitution in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)

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Electrospun carbon nanofiber-supported V_(2)O_(3) with enriched oxygen vacancies as a free-standing high-rate anode for an all-vanadium-based full battery

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Carbon Energy 2024年第9期6卷 15-28页

作者： Qi Lai Bincen Yin yu Dou Qing Zhang yunhai Zhu Yingkui Yang School of Chemistry and Materials Science South-Central Minzu UniversityWuhanChina State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhanChina

Synergistic regulation of hierarchical nanostructures and defect engineering is effective in accelerating electron and ion transport for metal oxide ***,carbon nanofiber-supported V_(2)O_(3) with enriched oxygen vacancies(ov-V_(2)O_(3)@CNF)was fabricated using the facile electrospinning method,followed by thermal *** from the traditional particles embedded within carbon nanofibers or irregularly distributed between carbon nanofibers,the free-standing ov-V_(2)O_(3)@CNF allows for V_(2)O_(3) nanosheets to grow vertically on one-dimensional(1D)carbon nanofibers,enabling abundant active sites,shortened ion diffusion pathway,continuous electron transport,and robust structural ***,density functional theory calculations confirmed that the oxygen vacancies can promote intrinsic electron conductivity and reduce ion diffusion energy ***,the ov-V_(2)O_(3)@CNF anode delivers a large reversible capacity of 812 mAh g^(-1) at 0.1 A g^(-1),superior rate capability(405 mAh g^(-1) at 5 A g^(-1)),and long cycle life(378 mAh g^(-1) at 5 A g^(-1) after 1000 cycles).Moreover,an all-vanadium full battery(V2O5//ov-V_(2)O_(3)@CNF)was assembled using an ov-V_(2)O_(3)@CNF anode and a V2O5 cathode,which outputs a working voltage of 2.5 V with high energy density and power density,suggesting promising practical *** work offers fresh perspectives on constructing hierarchical 1D nanofiber electrodes by combining defect engineering and electrospinning technology.

关键词： electrospun electrode full battery oxygen vacancy vanadium trioxide

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How interfacial electron-donating defects influence the structure and charge of gold nanoparticles on TiO_(2)support

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Nano Research 2024年第7期17卷 5965-5974页

作者： Guang-Jie Xia yu Fu Wei Cao Jun Li Yang-Gang Wang Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055China School of Physical Sciences Great Bay UniversityDongguan 523000China Department of Chemistry Tsinghua UniversityBeijing 100084China

The reduction degree of TiO_(2)support is critical to the performances of metal *** many previous theoretical calculations,only the bridge oxygen vacancy(ov)was considered as the electron-donating defect on reduced rutile TiO_(2)(r-TiO_(2−x))***,titanium adatoms(Tiad.),oxidized titanium islands(***),and acid hydroxyls(ObrH)also exist at the metal/support *** conducting density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations,we compared r-TiO_(2−x)surfaces with ov,Tiad.,***,and ObrH sites loaded with Au nanoparticles(NPs).The results showed the Au NPs were oxygen-phobic but titanium-philic,resulting in wetting of ov and *** short contact with *** and *** Bader charges of Au NPs(QM)showed a good linear relationship with the ideal number of donating electrons(Ne)from the defective sites(QM=−KeNe+QM,S),demonstrating the intrinsic electron allocation at the *** ov,Tiad.,and *** exhibited similar slopes(Ke),relatively steeper than that of *** means in the scope of Au NP charge state,the *** *** have a close electron-donating ability with ov,but the ObrH donates relatively fewer *** linear relationship can be extended approximately to other *** higher the metal work function,the steeper the Ke for easier electron donation from defective *** stronger the metal oxygen affinity,the more positive the intercept(QM,S).That explains the easy generation of metallic or negative Pt and Au NPs on r-TiO_(2−x),but hard for Cu and Zn in *** provides theoretical guidance for regulating the charge of metal NPs over TiO_(2−x)supports.

关键词： metal-support interaction titanium oxide oxygen vacancy surface hydroxyl titanium adatom

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Impact of uterine artery embolization on ovarian function and pregnancy outcome after uterine-fibroids treatment:A prospective study

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World Journal of Clinical Cases 2024年第15期12卷 2551-2559页

作者： Jing-Lei Liu Zhi-Hui Liang Bao Cui Jian-yu Liu Li Sun Department of Interventional Treatment 980(Bethune International Peace)Hospital of PLA Joint Logistics Support ForcesShijiazhuang 050082Hebei ProvinceChina Department of Obstetrics and Gynecology 980(Bethune International Peace)Hospital of PLA Joint Logistics Support ForcesShijiazhuang 050082Hebei ProvinceChina

Uterine fibroids are benign tumors that originate from smooth muscle cells of the *** is the most common gynecological disorder,affecting up to 80%of women of reproductive *** fibroids can cause various symptoms such as abnormal uterine bleeding,pelvic pain,infertility,and pregnancy *** treatment options for uterine fibroids include medical therapy,surgical intervention,and minimally invasive *** To compare ovarian function of women with uterine fibroids who did or did not undergo uterine artery embolization(UAE).METHODS This prospective cohort study enrolled 87 women with symptomatic uterine fibroids who underwent UAE,and 87 women with the same symptoms who did not undergo UAE but received conservative management or other *** two groups were matched for age,body mass index,parity,and baseline characteristics of uterine *** primary outcome was ovarian function that was evaluated by serum levels of follicle-stimulating hormone(FSH),luteinizing hormone(LH),estradiol(E2),and anti-Müllerian hormone(AMH),as well as ovarian reserve tests,such as antral follicle count(AFC)and ovarian volume(ov).The secondary outcome was fertility that was evaluated based on the menstrual cycle,ovulation,conception,pregnancy,and *** participants were followed-up for 36 months and assessed at 1,3,6,12,24,and 36 months after *** The study found that the most common minor complication of UAE was postembolization syndrome in 73.6% of women,resolving within a *** significant differences were observed between the UAE group and the control group in serum levels of reproductive hormones(FSH,LH,E2,AMH)and ovarian reserve indicators(AFC,ov)at any point up to 36 months ***,there were no significant differences in conception,pregnancy,or delivery rates,with the average time to conception and gestational age at delivery being similar between the two *** weights were also ***

关键词： Uterine fibroids Uterine artery embolization ovarian function Fertility Pregnancy outcome Embolic agent

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Integrating Zeolite and Layered Double Hydroxide for Highly Selective Catalytic Production ofγ-Valerolactone

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CCS Chemistry 2024年第3期6卷 652-662页

作者： Mingkun Gao Guoju Yang Guangyuan He Risheng Bai Jialiang Li Yinghao Liu Qiang Zhang Guangrui Chen Donghai Mei Jihong yu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryInternational Center of Future ScienceJilin UniversityChangchun 130012 School of Materials Science and Engineering Tiangong UniversityTianjin 300387

The production ofγ-valerolactone(GVL)from biomass derivatives levulinic acid(LA)based on acidbase metallic catalysts offers a sustainable pathway to the synthesis of valuable chemicals and ***,the development of efficient metallic catalysts with tunable Lewis acid–base and Brønsted acid sites remains a ***,for the first time,we integrated zeolite and layered double hydroxide(LDH),in a core–shell structure,wherein zeolite and CoFe-LDH provided the Brønsted acidic sites and Lewis acid sites,***,oxygen vacancies(ov_(x))acting as Lewis bases were generated on the surface of LDH via Ga *** efficient cascade catalytic reaction from LA to GVL was successfully achieved over the designed Beta@LDH-ovx catalyst,affording a superior conversion of LA(>99.9%)and an impressive selectivity to GVL(89.18%).Importantly,the“memory effect”of LDH endowed the catalyst with excellent regeneration of metal active *** functional theory calculations revealed that the introduced ovx facilitated the adsorption of carbonyl oxygen in LA and boosted the production of GVL through the synergistic effect of acid/base sites in the composite *** work presents a rational design route for the construction of multifunctional catalysts by coupling zeolites and LDHs for highly selective catalytic conversion of biomass.

关键词： zeolite layered double hydroxide oxygen vacancies biomass γ-valerolactone

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A COMPREHENSIVE STUDY OF FRETTING FATIGUE OF STRUCTURAL ALLOYS IN SYMMETRIC TENSION-COMPRESSION

A COMPREHENSIVE STUDY OF FRETTING FATIGUE OF STRUCTURAL ALLO...

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第三届摩擦疲劳学国际会议

作者： G.V. TSYBAN’ov yu. KURASH Institute for Problems of Strength National Academy of Sciences of Ukraine 2 Timiryazevskaya str. Kiev-14 01014 Ukraine Institute for Problems of Strength National Academy of Sciences of Ukraine 2 Timiryazevskaya str. Kiev-14 01014 Ukraine

＜正＞A method of fatigue testing is proposed for fretting pairs of structural alloys. The distinctive feature of the method is a possibility of measuring and controlling contact pressure, friction forces, and sliding amplitudes using electric signals with a subsequent preliminary processing, filtering and accumulation of the tests results in a computer. The authors justify the use of the value of electrie microcurrents occurring in the fretting pair in the course of testing as a parameter for the evaluation of the level of damaging processes of nonmechanical nature.

关键词： Fretting fatigue Damaging processes Tribocurrents Data processing

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木质素磺酸钙增强花岗岩残积土微生物固化效果研究

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土木工程学报 2024年第3期57卷 123-132页

作者：朱文羲邓华锋李建林肖瑶熊雨程雷三峡大学三峡库区地质灾害教育部重点实验室湖北宜昌443002 三峡大学土木与建筑学院湖北宜昌443002

为提升微生物固化花岗岩残积土的效果,综合考虑木质素磺酸钙的特点和MICP(Microbial-induced calcite precipitation)作用过程的环境条件,设计进行木质素磺酸钙增强MICP固化花岗岩残积土试验,综合宏观物理力学试验和微细观检测,系统分... 详细信息

为提升微生物固化花岗岩残积土的效果,综合考虑木质素磺酸钙的特点和MICP(Microbial-induced calcite precipitation)作用过程的环境条件,设计进行木质素磺酸钙增强MICP固化花岗岩残积土试验,综合宏观物理力学试验和微细观检测,系统分析木质素磺酸钙对微生物固化花岗岩残积土的增强效果及增强机制。结果表明:①木质素磺酸钙能够显著提高花岗岩残积土微生物加固过程中的胶结物产量,木钙掺量在4.00%左右达到最佳,与常规MICP相比,胶结物生成量提高了48.86%;②木质素磺酸钙的掺入,显著提高了固化体的抗压强度和抵抗变形能力,2.00%~8.00%掺量下固化体的抗压强度提升了4.75%~41.20%,破坏时应变增加16.24%~38.55%;③掺入木质素磺酸钙后,固化体的孔隙大小及孔隙率均有不同程度降低,孔隙率降低了12.97%~37.38%,固化体的整体密实性进一步增强;④木质素磺酸钙的掺入,改善了残积土的孔隙结构,为后续微生物加固提供更好的环境条件;⑤在微生物固化花岗岩残积土过程中掺入木质素磺酸钙后,改善了微生物生长的酸碱环境,丰富了MICP作用过程中的钙源,提升了固菌率,促进了MICP反应,同时改善了碳酸钙沉淀颗粒的大小、性状及排列形式,使得胶结物产量进一步提升,从而提升固化体的整体固化效果。

关键词：木质素磺酸钙 MICP 花岗岩残积土固化效果微观结构

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Hydrogen evolution activity enhancement by tuning the oxygen vacancies in self-supported mesoporous spinel oxide nanowire arrays

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Nano Research 2018年第2期11卷 603-613页

作者： Dali Liu Chao Zhang Yifu yu Yanmei Shi yu yu Zhiqiang Niu Bin Zhang Department of Chemistry School of Science and Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin University Tianjin China Collaborative Innovation Center of Chemical Science and Engineering Tianjin China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin China

The development of facile strategies to tune the oxygen vacancy （ov） content in transition metal oxides （TMOs） is paramount to obtain low-cost and stable electrocatalysts, but still highly challenging. Taking NiC0204 as a model system, we have experimentally established a facile calcination and electrochemical activation （EA） methodology to dramatically increase the concentration of ovs and provide theoretical insight into how the concentration of ovs affects the performance of spinel TMOs towards the electrochemical hydrogen evolution reaction （HER）. A self-supported cathode of ov-rich NiC0204 nanowire arrays was found to exhibit higher HER activity and better stability in alkaline media than its counterparts with fewer ovs. The electrocatalytic HER activity was in good agreement with the increasing concentration of ovs in the studied samples. A large current density of 360 ***-2 was reached with an overpotential of only 317 mV. Additionally, such a facile strategy was able to efficiently generate ovs in other TMOs （e.g., CoFe204 and NiFe204） for enhanced HER performance. In addition, our theoretical results suggest that the increasing ov concentration reduces the adsorption energy of water molecules and their dissociation energy barrier on the surface of the catalyst, thus leading to performance improvement of spinel TMOs toward the electrochemical HER. This work may open a new avenue to increase the concentration of ovs in TMOs in a controlled manner for promising applications in a variety of fields.

关键词： electrochemical activation,hydrogen evolutionreaction,oxygen vacancy spinel phase,thermal treatment

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嘌呤能受体在卵巢癌中的预后价值及肿瘤免疫浸润分析

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医学信息 2024年第17期37卷 1-10页

作者：李朝周玉明姜茹于运亮临清市人民医院检验科滨州医学院烟台附属医院检验科

目的构建浆液性卵巢癌（ov）嘌呤能受体家族基因的预后模型，分析基因的表达与免疫细胞浸润及常用化疗药物的关系。方法下载癌症基因图谱（TCGA）等数据库中15个嘌呤能受体家族基因的表达谱数据及临床信息，利用LASSO回归分析筛选与O... 详细信息

目的构建浆液性卵巢癌（ov）嘌呤能受体家族基因的预后模型，分析基因的表达与免疫细胞浸润及常用化疗药物的关系。方法下载癌症基因图谱（TCGA）等数据库中15个嘌呤能受体家族基因的表达谱数据及临床信息，利用LASSO回归分析筛选与ov患者生存有关的基因，根据风险值对患者分组并使用Kaplan-Meier Plotter对关键基因进行生存分析。应用多因素Cox回归分析构建基于TCGA-ov数据集的预后模型，绘制列线图和校准曲线。利用TIMER、xCell算法进行免疫浸润分析。利用TIDE算法分析基因的表达与免疫检查点阻断（ICB）治疗的相关性。利用TCGA联合癌症药物敏感性基因组学（GDSC）数据库进行药物敏感性分析。结果 LASSO回归分析筛选得到6个嘌呤能受体家族基因与ov患者预后有关。多因素Cox回归分析显示，P2RX6、P2RY12、P2RY14、年龄和种族是ov患者独立的预后因素（Pov中表达下调（Pov患者的预后模型，经筛选得出P2RY14可作为ov患者预后独立危险因素，可为指导ov的免疫治疗提供新的思路和方向。

关键词：嘌呤能受体浆液性卵巢癌数据库预后免疫浸润

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Interactions between Bioactive Diperoxovanadate Complexes and Imidazole: Insights into Their Solution Structures by NMR and ESI-MS

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Chinese Journal of Structural Chemistry 2004年第6期23卷 511-518页

作者： yu Xian-Yong CAI Shu-Hui CHEN Zhong Departments of Physics and Chemistry State Key Laboratory for Physical Chemistry of Solid SurfaceXiamen UniversityXiamen 361005China State Key Laboratory of Structural Chemistry Fuzhou 350002China

The interactions between four high bioactive diperoxovanadate complexes Kn[ov(O2)2L]mH2O (n = 1~3, m = 1~5, L = oxalate (abbr. oxa), picolinate (abbr. pic), bipyridine (abbr. bipy) and 1,10-phenanthroline (abbr. phen); their corresponding complexes abbreviated as bpV(oxa), bpV(pic), bpV(bipy) and bpV(phen), respectively) and imidazole (abbr. imi) in solution were studied by several NMR techniques: multinuclear (1H, 13C and 51V) and variable temperature 51V NMR. Competitive coordination interactions were observed and the order of the interaction strength of the four complexes with imidazole is as follows: bpV(oxa) > bpV(pic) > bpV(bipy) > bpV(phen), which is deeply affected by the identity of the ligands and has the same order as their inhibition effect toward bovine heart phosphotyrosyl protein phosphatase. The species [ov- (O2)2(imi)]- was formed in all cases. Both of the NMR data and equilibrium constants of the interaction systems were reported. The experimental results indicate that the species of bpV(oxa) and [ov(O2)2(imi)]- are six-coordinated, while bpV(pic), bpV(bipy) and bpV(phen) are seven- coordinated in solution. ESI-MS results support the conclusions obtained by NMR.

关键词： diperoxovanadate imidazole interaction NMR ESI-MS

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