High-Index Faceted Nanocrystals as Highly Efficient Bifunctional Electrocatalysts for High-Performance Lithium-Sulfur Batteries

Precisely regulating of the surface structure of crystalline materials to improve their catalytic activity for lithium polysulfides is urgently needed for high-performance lithium-sulfur(Li-S)batteries.Herein,high-index faceted iron oxide(Fe_(2)O_(3))nanocrystals anchored on reduced graphene oxide are developed as highly efficient bifunctional electrocatalysts,effectively improving the electrochemical performance of Li-S batteries.The theoretical and experimental results all indicate that high-index Fe_(2)O_(3)crystal facets with abundant unsaturated coordinated Fe sites not only have strong adsorption capacity to anchor polysulfides but also have high catalytic activity to facilitate the redox transformation of polysulfides and reduce the decomposition energy barrier of Li_(2)S.The Li-S batteries with these bifunctional electrocatalysts exhibit high initial capacity of 1521 mAh g^(-1)at 0.1 C and excellent cycling performance with a low capacity fading of 0.025%per cycle during 1600 cycles at 2 C.Even with a high sulfur loading of 9.41 mg cm^(-2),a remarkable areal capacity of 7.61 mAh cm^(-2)was maintained after 85 cycles.This work provides a new strategy to improve the catalytic activity of nanocrystals through the crystal facet engineering,deepening the comprehending of facet-dependent activity of catalysts in Li-S chemistry,affording a novel perspective for the design of advanced sulfur electrodes.

High-index faceted noble metal nanostructures drive renewable energy electrocatalysis

Noble metallic nanocrystals are used in a wide variety of applications,such as catalysis,batteries,and bio-and chemical sensors.Most of the previous studies focus on the preparation of thermodynamically stable nanocrystals enclosed by low-index facets and discuss their corresponding catalytic properties.Recently,researchers have found that the nanocrystals with high-index facets(HIFs)are of more interest for electrocatalysis.Herein,we review recent key progress in the synthesis of noble metallic nanoparticles enclosed with HIFs and their facetdependent electrocatalytic behaviors.First,we introduce the concept of HIFs,and establish the correlation between their surface structure and catalytic activity.Then,we discuss various synthetic approaches for controlling the shapes and composition of the nanocrystals enclosed by HIFs.Afterwards,we showcase the enhanced electrocatalytic performance realized by HIF-based nanostructures.Finally,we provide guidance on how to improve the electrocatalysis by engineering HIFs on noble metallic nanocrystals.

Compact and high-efficient wavelength demultiplexing coupler based on high-index dielectric nanoantennas

Wavelength demultiplexing waveguide couplers have important applications in integrated nanophotonic devices. Two of the most important indicators of the quality of a wavelength demultiplexing coupler are coupling efficiency and splitting ratio. In this study, we utilize two asymmetric high-index dielectric nanoantennas directly positioned on top of a silicon-on insulator waveguide to realize a compact wavelength demultiplexing coupler in a communication band, which is based on the interference of the waveguide modes coupled by the two nanoantennas. We add a Au substrate for further increasing the coupling efficiency. This has constructive and destructive influences on the antenna＇s in-coupling efficiency owing to the Fabry-Perot（FP） resonance in the SiO2 layer. Therefore, we can realize a wavelength demultiplexing coupler with compact size and high coupling efficiency. This coupler has widespread applications in the areas of wavelength filters,on-chip signal processing, and integrated nanophotonic circuits.

Four-wave mixing in silicon-nanocrystal embedded high-index doped silica micro-ring resonator

A nonlinear integrated optical platform that allows the fabrication of waveguide circuits with different material composition,and at small dimensions,offers advantages in terms of field enhancement and increased interaction length,thereby facilitating the observation of nonlinear optics effects at a much lower power level.To enhance the nonlinearity of the conventional waveguide structure,in this work,we propose and demonstrate a microstructured waveguide where silicon rich layer is embedded in the core of the conventional waveguide in order to increase its nonlinearity.By embedding a 20 nm thin film of silicon nanocrystal(Si-nc),we achieve a twofold increase of the nonlinear parameter,γ.The linear relationship between the fourwave mixing conversion efficiency and pump power reveals the negligible nonlinear absorption and small dispersion in the micro-ring resonators.This simple approach of embedding an ultra-thin Si-nc layer into conventional high-index doped silica dramatically increases its nonlinear performance,and could potentially find applications in all-optical processing functions.

Co_(2)P nanorods with exposure of high-index facets for efficient photochemical reduction of CO_(2)by promoting the directional transfer of electrons

Herein,Co_(2)P nanorods(NRs)with exposure to high-index facets(HIFs)were prepared by a special assembly-calcination method using thioacetamide(TAA)as a structure-directing reagent.The analysis of adsorption energies of S atoms on different facets as well as the surface energies of Co_(2)P indicate that the HIFs become more stable after adsorbing S atoms.With rich unsaturated sites on HIFs,the photochemical reduction rate of CO_(2)over Co_(2)P NRs is 14.5 mmol h^(-1)g^(-1)for the production of CO within 3 h.The analysis of electron transfer,bond lengths,bond angles and adsorption energies indicate that the CO_(2)molecules are more easily adsorbed and activated on the HIFs.The free energy calculations and d band theory demonstrate that the HIFs are conducive to reducing the formation energy barriers as well as improving the stability of the intermediate^(*)COOH,then enhancing the catalytic performance of CO_(2)reduction.

Tunning the bandgap of MnO_(2)homojunction by building active high-index facet to achieve rapid electron transfer for enhanced photocatalytic sterilization

Photocatalysis has been a research hotspot in recent years,and the design and modification of photocat-alysts have been the key points.Common methods for designing photocatalysts,including constructing heterojunctions and homojunctions,have been developed on the basis of heterojunctions.In this study,two homojunctions of manganese dioxide(MnO_(2)),including a high-index crystal plane homojunction and a general homojunction,are prepared using a stepwise hydrothermal method.Using a capping agent,the high-index crystal surface of the MnO_(2)is exposed.It is found that the electron transport efficiency be-tween the two components of the homojunction with high-index planes is higher and the adsorption capacity of the oxygen is stronger,which leads to higher photocatalytic efficiency.In addition,the newly designed high-index homojunction is used for the treatment of bacterial infections,and it kills Staphy-lococcus aureus(S.aureus)and Escherichia coli(E.coli)at rates of 99.95%±0.04%and 99.31%±0.25%,respectively.It also has excellent therapeutic effects on mouse wounds,which implies superb practical application value.This work provides a new strategy for the improved design of homojunctions and the application of photocatalytic materials.

Mg-doped CaCO_(3)nanoarchitectures assembled by(441)high-index facets for efficient trace removal of Pb(Ⅱ)

Removal of trace heavy metal ions puts high demands on designing adsorbents with favorable surfaces.Crystal-plane engineering can provide controllable adsorption energy between surficial planes and adsorbents.Herein,we have creatively synthesized Mg-doped CaCO_(3)nanoarchitectures assembled by layered sheets(Mg-CaCO_(3)LSs)with high-index facets of(441)through a facile wet chemical process.Adsorption tests reveal that the layer-bylayer assembled sample exhibits a maximum Pb(II)adsorption capacity of 1961.9 mg·g^(-1),agreeing with the monolayer-adsorption Langmuir model.At an initial Pb(II)ion concentration of 20 mg·L^(-1),the adsorption can achieve a high removal rate near 99.0%within 1 min,and the adsorption kinetics follows a chemisorption pseudo-second-order model.Interestingly,the Mg-CaCO_(3)LSs show much-improved adsorption properties towards low-concentration Pb(II)ions,which could reduce the concentration from 1 mg·L^(-1)to~2.9μg·L^(-1)in 3 h(within 30 min decrease to less than 10μg·L^(-1),meeting drinking water standard from WHO).For comparison,the commercial CaCO_(3)and collected CaCO_(3)scale show much lower adsorption values with Pb(Ⅱ)ion residual concentration of~935.0 and~944.9μg·L^(-1)in 3 h,respectively.Xray diffraction(XRD),energy dispersive spectroscopy(EDS),and inductively coupled plasma(ICP)characterizations on the Mg-CaCO_(3)LSs before and after adsorbing Pb(Ⅱ)confirm that the high removal performance could be ascribed to fast metal ion exchange and excellent physical adsorption contributed by high-index planes.The density functional theory(DFT)calculations also confirm that the much-enhanced adsorption kinetics benefits from the optimal adsorption of the(441)planes.This work will provide a feasible route to design highefficient low-cost adsorbents through crystal-plane engineering.

Shape transformation of gold nanoparticles in aqueous CTAB/CTAC solution to generate high-index facets for electrocatalysis and SERS activity

Gold nanoparticles(Au NPs)have demonstrated great potential in chemical and biological sensing,catalysis,biomedicine,X-ray computed tomography,and other applications,owing to their unique properties.Au NPs with high-index facets have attracted more attention in the past decade owing to their superior electrocatalytic activity in fuel cells and enhanced performance in surface-enhanced Raman spectroscopy(SERS)applications.This review presents an overview of our achievements in the direct synthesis of Au NPs with controlled shapes in water using cationic surfactants.By deliberately adjusting the nature of the surfactant stabilizers,preformed Au NPs with simple shapes can be readily transformed into Au NPs with complicated shapes with controlled high-index facets by simple seeded growth.The high-index facets of the as-prepared Au NPs can be consistently correlated with their superior performance in the electrooxidation of methanol and ethanol and their enhanced SERS activity.

Deterministic Synthesis of Pd Nanocrystals Enclosed by High-Index Facets and Their Enhanced Activity toward Formic Acid Oxidation

Noble-metal nanocrystals enclosed by high-index facets are of growing interest due to their enhanced catalytic performance in a variety of reactions.Herein,we report the deterministic synthesis of Pd nanocrystals encased by high-index facets by controlling the rate of deposition(V_(deposition))relative to that of surface diffusion(V_(diffusion)).For octahedral seeds with truncated corners,a reduction rate(and thus deposition rate)faster than that of surface diffusion(i.e.,V_(deposition)/V_(diffusion)>1)led to the formation of concave trisoctahedra(TOH)with high-index facets.When the reduction was slowed down,in contrast,surface diffusion dominated the growth pathway.In the case of V_(deposition)/V_(diffusion)≈1,truncated octahedra with enlarged sizes were produced.When the reduction rate was between these two extremes,we obtained concave tetrahexahedra(THH)without or with truncation.Similar growth patterns were also observed for the cuboctahedral seeds.When the Pd octahedra,concave TOH,and concave THH were tested for electrocatalyzing the formic acid oxidation(FAO)reaction,those with high-index facets were advantageous over the conventional Pd octahedra enclosed by{111}facets.This work not only contributes to the understanding of surface diffusion and its role in nanocrystal growth but also offers a general protocol for the synthesis of nanocrystals enclosed by high-index facets.

口岸经济高质量发展水平评价指标体系构建与测度——基于云南的实证研究

加快口岸由“通道经济”转型为“产业经济”,是“一带一路”建设高质量发展的重要内容。基于高质量发展目标要求,对口岸经济高质量发展的内涵、特征进行学理性探讨,依托层次分析思想构建测度口岸经济高质量发展水平的评价指标体系。以边境口岸数量多、类型丰富的云南省为研究对象,选取2012—2021年数据,运用CRITIC权重法,对云南口岸经济高质量发展水平进行测度并分析其趋势特征。研究发现:样本期内云南口岸经济高质量发展水平总体呈现上升趋势,口岸经济协调发展和开放发展提升显著,创新发展有待加强,共享作用显现,绿色发展不平稳,岸城协调性不足。推动云南口岸经济高质量发展要转变发展理念,扩大高水平对外开放,建立岸岸、岸城协调发展机制,完善口岸基础设施,加强口岸开放发展能力,以此推进云南口岸现代化建设进程。

高质量发展视域下美国生涯与技术教育评价指标体系构建与启示

为实现高质量发展目标,美国生涯与技术教育亟需考察经费投入效果,转变问责评价重点,并构建了以“评价维度—评价要素—评价标准”为核心的三级评价指标体系。该指标体系具有评价维度立足多视角和全方位,评价要素体现全纳性和公平性,评价标准重视以学生为中心等特征。借鉴其基本思路,我国职业教育评价指标体系的构建,需树立全面的高质量评价观、关注多元化的评价主体需求、设计以人为本的评价内容。

身体质量指数联合三酰甘油与高密度脂蛋白胆固醇比值预测2型糖尿病风险

目的利用体检指标中身体质量指数(BMI)和三酰甘油与高密度脂蛋白胆固醇比值(triglyceride to high-density lipoprotein cholesterol,TG/HDL-C)联合预测2型糖尿病(type 2 diabetes mellitus,T2DM)发病风险。方法基于瑞慈医疗集团2010—2016年体检人群的数据库,通过Cox比例风险模型观测不同BMI的人群基线TG/HDL-C对随访期间T2DM风险的影响,并分析TG/HDL-C与BMI是否存在交互作用。结果在随访期间,13685例研究对象中共有315例最终诊断为T2DM。以BMI=24 kg/m^(2)为界,将所有研究对象分成两个亚组。BMI<24 kg/m^(2)的亚组共有8238例研究对象,96例在随访结束时患T2DM,对潜在的混杂因素进行调整后,升高的TG/HDL-C导致T2DM事件的风险较高[HR 95%CI=1.47(1.23,1.74),P<0.001]。与最低五分位数(Q1)相比,升高的TG/HDL-C五分位数(Q2~Q5)T2DM发病率增加[HR 95%CI分别为:0.73(0.28,1.93)、2.75(1.29,5.85)、2.81(1.28,6.20)和3.91(1.51,10.11)]。BMI≥24 kg/m^(2)的亚组共有5447例研究对象,219例在随访结束时患T2DM。在两个亚组中,随着TG/HDL-C的增加,T2DM患病风险均呈非线性增加,这一变化在BMI<24 kg/m^(2)的亚组更为明显。绘制两个亚组TG/HDLC与3年和5年T2DM发病的ROC曲线,在BMI<24 kg/m^(2)的亚组中,ROC曲线下面积分别为0.72和0.77。在BMI≥24 kg/m^(2)的亚组中,ROC曲线下面积则分别为0.55和0.57。结论在BMI<24 kg/m^(2)的人群中,TG/HDL-C的升高提示T2DM患病风险显著增加。

三级公立医院绩效考核背景下加强高校附属医院高质量发展的思考

三级公立医院绩效考核是检验公立医院医疗综合能力和水平的“金标准”。学科建设是高校附属医院实现高质量发展的关键。本研究对比分析了三级公立医院绩效考核与世界大学学科排名、学科评估指标体系差异情况,探讨了如何通过国家、高校和附属医院三方努力,共同引导高校附属医院加强学科建设,持续提升综合实力和国际竞争力,为探索中国特色世界一流大学附属医院高质量内涵式发展提供参考路径。

CMA-GEPS极端温度预报指数及2022年夏季极端高温预报检验评估

极端预报指数(EFI)是利用集合预报获取极端天气信息的有效工具之一。为提升CMA全球集合预报系统(CMAGEPS)对极端天气的预报能力,针对CMA-GEPS历史预报数据少且再预报数据缺乏、难以合理统计模式气候分布的难题,研究利用小样本确定性预报数据形成EFI所需模式气候分布的方法。采用2020年6月15日—2022年7月22日CMA全球高分辨率(0.25°×0.25°)确定性业务预报数据,通过一种时间、空间样本扩展方法建立了与较低分辨率(0.5°×0.5°)的CMA-GEPS预报模式版本匹配的各预报时效(1—10 d)逐月模式气候分布。使用CMA-GEPS业务预报和ERA5再分析数据评估了CMA-GEPS 2 m气温EFI对2022年夏季(6—8月)中外4个代表性区域极端高温的预报能力。基于相对作用特征曲线的检验结果表明,CMA-GEPS EFI在1—10 d的短、中期预报时效上均具备区分极端高温的能力。以最大TS评分为准则,确定了用于发布极端高温预警信号的EFI临界阈值。EFI的预报能力随预报时效延长呈下降趋势,且在不同区域的表现存在差异:对中国长江中下游地区极端高温的预报能力在各时效上均优于华北地区;欧洲西部地区1—7 d时效上的EFI预报能力高于欧洲中部地区,而欧洲中部地区8—10 d时效上的EFI预报能力更好。上述结果与2 m气温的集合预报质量随预报时效与空间位置而变化有关。经济价值模型的评估结果表明,基于EFI预报信息的风险决策存在一定的经济价值和参考价值。个例分析结果进一步展现了CMA-GEPS EFI能够在中期预报时效上发出极端高温早期预警的能力。

补饲胆固醇对高温环境下湖羊母羊繁殖性能和血清生化指标的影响

【目的】研究饲粮中添加胆固醇对中国南方夏季湖羊发情率、受胎率和血清生化指标的影响。【方法】选择108只体重相近(33.60 kg±1.86 kg)的健康湖羊母羊,其中30只湖羊在非高温季节(4月份,平均最高温度20.9℃±3.2℃)饲粮添加不同剂量胆固醇(0.1%和0.5%),ELISA方法检测血清中胆固醇含量的动态变化,筛选合适的胆固醇添加量;另外78只湖羊随机分成2组(对照组和试验组),试验期63 d(从同期发情处理第1天到自然发情后配种的第30天),在夏季高温季节(7-9月份,平均最高温度31.3℃±2.6℃),对照组饲喂基础饲粮,试验组饲喂添加0.1%胆固醇的基础饲粮,ELISA方法检测血清中雌二醇(E2)和孕酮(P4)水平,研究饲粮添加胆固醇对湖羊发情率、受胎率和血清生化指标的影响。【结果】非高温季节湖羊基础饲粮中分别添加0.1%和0.5%胆固醇,48 h后两组湖羊血清中胆固醇含量趋于一致,据此选择0.1%作为高温季节补饲胆固醇的添加剂量。夏季高温季节在补饲0.1%胆固醇的第3、30和63天均能显著提高湖羊血清中胆固醇含量(P<0.05);且试验组湖羊自然发情率(89.7%)高于对照组(82.1%)(P>0.05),受胎率(60.0%)显著高于对照组(46.9%)(P<0.05)。试验组湖羊总蛋白、球蛋白、白细胞介素-1和甘油三酯含量均显著高于对照组(P<0.05),而尿素氮含量显著下降(P<0.05)。【结论】夏季高温环境下,在湖羊母羊饲粮中添加0.1%胆固醇可有效提高其发情率和受胎率。

绿色金融赋能河南省经济高质量发展对策研究

为深入探究绿色金融与经济高质量发展之间的相互关系,充分发挥金融对经济发展的促进作用,从绿色信贷、绿色债券、绿色保险、绿色投资等四个维度构建绿色金融发展评价指标体系,从发展规模和效率、协调、绿色、开放、共享等五个维度构建经济高质量发展评价指标体系。选用2017—2020年河南省18个城市面板数据为研究基础,深入研究绿色金融与经济高质量发展之间的耦合协调关系,并结合河南省省情特点,提出绿色金融赋能河南省经济高质量发展的对策建议。

广东省三级综合医院优质护理服务评价指标的构建

目的构建广东省三级综合医院优质护理服务评价指标,为促进优质护理服务评价工作和规范优质护理服务提供参考。方法基于文献检索的基础上,应用头脑风暴法并借鉴国内已有的相关制度、标准和政策构建出评价指标条目池和问卷初稿;采用德尔菲法对评价指标进行两轮专家函询。结果两轮专家函询的回收率分别为80.00%和91.67%;权威程度系数均为0.93,医院部分Kendall协调系数W分别为0.128和0.116,病区部分分别为0.193、0.107,差异具有统计学意义(均P<0.001)。第2轮函询医院各指标的重要性均数为(4.43~5.00)分。第2轮函询病区各指标的重要性均数为(4.59~5.00)分。构建的广东省三级综合医院优质护理服务评价指标包括医院和病区两个部分,其中医院部分包括一级指标8项、二级指标22项、三级指标65项,病区部分包括一级指标9项、二级指标23项、三级指标50项。结论本研究编制的广东省三级综合医院优质护理服务评价指标具有较好的科学性和可靠性,有利于完善优质护理服务管理制度,引导优质护理服务健康发展。

新时代高职教育高质量发展评价指标体系构建及推进路径研究

从协调发展、产教融合、供需适配、育人质量、国际影响五个维度构建了5个一级指标,11个二级指标,43个观测点的新时代高职教育高质量发展评价指标体系,并利用专家排序法确定了指标的权重。以评价体系所界定的维度为导引,探讨了推动职业教育高质量发展需优化职业教育类型特色、培养高素质技能型人才、职业教育供给与经济发展需求匹配、切实提升教育教学质量、构建职业教育开放体系。

常州市主城区高强度降水变化特征及其影响分析

以常州市主城区为研究区域,基于高强度降水指数等指标,分析常州市主城区高强度降水特性及其对城市防汛的影响。研究结果表明,受气候变化和城镇化等影响,常州市主城区在1953—2022年期间有雨日数等3个极端降水日数指标、强降水量等6个高强度降水量级指标均呈递增趋势。

Fe稳固的FeOOH@NiOOH电催化剂的大电流极化设计与析氧研究

电解水技术是制取高纯度氢气的有效途径,为传统的氢气生产提供了一种可持续的替代方案.其中,开发性能优异的电催化材料是降低电解水制氢成本的关键.析氧反应(OER)由于涉及多个电子转移而导致的动力学缓慢,是克服高过电位的主要挑战.镍铁羟基/氢氧化物(NiFe(oxy)hydroxides)是近期研究的热点,其在碱性条件下具有极低的OER过电位,部分材料性能甚至超过了贵金属基催化剂,如IrO_(2)和RuO_(2).然而,NiFe(oxy)hydroxides的长期催化稳定性,尤其是在大电流下的长期催化稳定性,成为限制其实际应用的主要问题,这主要是由于铁元素的严重流失导致的.因此,如何有效控制和利用电化学溶解/沉积动力学成为稳定铁位点的关键.为克服该挑战,本文提出了一种大电流极化重构方法来固定活性铁位点.通过在大电流(1.5 A cm^(-2))下对材料进行表面快速极化重构,成功制备了FeOOH@NiOOH(eFNO_(L))电催化剂.eFNO_(L)不仅具有稳定的铁位点,还暴露出高指数晶面,因此eFNO_(L)同时展现出较好的OER催化活性和稳定性.同时,密度泛函理论计算结果表明,与具有低指数晶面的FeNiOOH相比,大电流极化工程制备的分相eFNO_(L)对铁位点表现出更高的结合能,可以有效抑制OER过程中的铁流失,且高指数晶面在改变速率决定步骤和减少吸附能垒上具有更大的优势.电化学测试结果表明,经过优化后的eFNO_(L)催化剂在产生100和500 mA cm^(-2)大电流密度仅需234和27 mV的过电位,并且具有较小的Tafel斜率(35.2 mV dec^(-1)).由于铁位点结合能的提高,eFNO_(L)催化剂在500 mA cm^(-2)的电流密度下能够稳定催化超过100 h,且仅有1.5%的性能衰减,优于近期报道的大多数镍铁基OER催化剂.综上,本文为开发高活性和高稳定性能的催化剂提供了一种有效的大电流电化学重构策略,在电解水制氢领域实现其工业化的大规模应用方面显示出巨大潜力,有望降低可持续电解水制氢成本.