Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

Strategies to achieve effective nitrogen activation

Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.

Habitat Suitability and Distribution Pattern Response to Global Climate Change in a Widespread Species,the Asiatic Toad(Bufo gargarizans)

The distribution and diversity of the species are closely related to the global climate.As the most widely distributed species of Bufonidae in China,the study of the distribution pattern and habitat suitability of the Asiatic toad under climate change can help us understand the reply pattern of Bufonidae habitat to climate change.Here,combined with the Maxent model and GIS technology,the effects of climate change on the distribution pattern and habitat suitability of the Asiatic toad were comprehensively analyzed.The results show that the rainfall during the wettest season(Bio16)and the mean temperature of the driest season(Bio9)have a considerable impact on the distribution of the Asiatic toad.In the next 30 to 50 years,across the overall spacial scale of the Chinese mainland,the habitat of the Asiatic toad will be primarily in the eastern part of China and less in south part,while its distribution area will expand to the midwest and northwest parts of China.Overall,the area in which it can be distributed will be reduced and suitable habitat will shift to some regions of higher latitude and elevation.In a word,we systematically analyzed the changes of the distribution pattern and habitat suitability of the Asiatic toad with climate change,and we aim to provide data on how climatic variation may impact amphibians.

Host Genetic Background Impacts Microbiome Composition in Newborn Alligator

Genetic factors play a key role in determination of the structure of the cloacal flora for newborn Chinese Alligators.We collected the cloacal microbiomes for 24 newborn Chinese Alligators from three different genetic backgrounds for 16S gene amplicon sequencing.The number of cloacal flora for the Chinese Alligators from different groups was comparable but differed structurally.There were variations in proportions of floral compositions at the phylum and family levels;however,the main difference was at the genus level.There were two significant differences in richness and evenness among the three groups.Non-metric multidimensional scaling NMDS analysis revealed that the 24 samples could be clearly divided into three categories based on their genetic backgrounds(stress=0.0244).Thus,we postulated that newborn Chinese Alligators with different genetic backgrounds have different immune strengths,which affects individual responses to environmental microorganisms.In summary,newborn Chinese Alligators from different genetic backgrounds exhibit variations in cloacal microbiome.

Ultrahigh Density of Atomic CoFe-Electron Synergy in Noncontinuous Carbon Matrix for Highly Efficient Magnetic Wave Adsorption

Improving the atom utilization of metals and clarifying the M–M’interaction is both greatly significant in assembling high-performance ultra-light electromagnetic wave-absorbing materials.Herein,a high-temperature explosion strategy has been successfully applied to assemble the hierarchical porous carbon sponge with Co–Fe decoration via the pyrolysis of the energetic metal organic framework.The as-constructed hybrid displays a superior reflection loss(RL)value of-57.7 d B and a specific RL value of-192 d B mg-1 mm-1 at 12.08 GHz with a layer thickness of 2.0 mm(loading of 15 wt%).The off-axis electron hologram characterizes the highly distributed numerous polarized nanodomain variable capacitors,demonstrating the dipole and interfacial polarization along the edges of the nanopores.More importantly,the X-ray absorption spectroscopy analysis verifies the mutual interaction between the metal cluster and carbon matrix and the electronic coupling responsible for the greatly improved electromagnetic wave absorption.

Engineering the Coordination Sphere of Isolated Active Sites to Explore the Intrinsic Activity in Single-Atom Catalysts

Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.

Polyoxometalate-Incorporated Host-Guest Framework Derived Layered Double Hydroxide Composites for High-Performance Hybrid Supercapacitor

Metal organic frameworks have been employed as high-performance layered double hydroxide(LDH)composite supercapacitor electrode materials but have shown unsatisfactory redox ability and stability.Herein,a host-guest CuMo-based polyoxomet-alate-based metal organic framework(POMOF)with copious electrochemically active sites and strong electrochemical redox activi-ties has been effectively coupled with POM-incorporated CoNi-LDH to develop a nanocomposite(NENU-5@CoNi-LDH)by a simple solvothermal method.The designed electrode shows a high specific capacity of 333.61 mAh·g^(-1) at 1 A·g^(-1).In addition,the novel hy-brid symmetric supercapacitor NENU-5@CoNi-LDH/active carbon(AC)demonstrated a high energy density of 80.8 Wh·kg^(-1) at a power density of 750.7 W·kg^(-1).Interestingly,the nanocomposite of NENU-5@CoNi-LDH exhibits an outstanding capacitance reten-tion of 79%after 5000 charge-discharge cycles at 10 A·g^(-1).This work provides a new strategy and will be the backbone for future energy storage research.

Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO_(2) Electroreduction at Low Overpotentials

Transition metal-based single-atom catalysts(TM-SACs)are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO_(2)reduction reaction.However,developing TM-SACs with high activity and selectivity at low overpotentials is challenging.Herein,a novel Fe-based SAC with Si doping(Fe-N-C-Si)was prepared,which shows a record-high electrocatalytic performance toward the CO_(2)-to-CO conversion with exceptional current density(>350.0 mA cm^(−2))and~100%Faradaic efficiency(FE)at the overpotential of<400 mV,far superior to the reported Fe-based SACs.Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO_(2)battery delivers an outstanding performance with a maximal power density of 2.44 mW cm^(−2)at an output voltage of 0.30 V,as well as high cycling stability and FE(>90%)for CO production.Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving^(*)CO intermediate desorption,inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO_(2)RR performance.This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on singleatom sites to improve their electrocatalytic performance.

Changes in soil carbon sequestration and soil respiration following afforestation on paddy fields in north subtropical China

Aims Although many studies have reported net gains of soil organic carbon(SOC)after afforestation on croplands,this is uncertain for Chinese paddy rice croplands.Here,we aimed to evaluate the effects of affores-tation of paddy rice croplands on SOC sequestration and soil respiration(R).Such knowledge would improve our understanding of the efctive-ness of various land use options on greenhouse gas mitigation in China.Methods The investigation was conducted on the Chongming Island,north subtropical China.Field sites were reclaimed from coastal salt marshes in the 1960s,and soils were homogeneous with simple land use:histories.SOC stocks and R,levels were monitored over one year in a paddy rice cropland,an evergreen and a deciduous broad-leaved plantation established on previous paddy fields and a reference fal-low land site never cultivated.Laboratory incubation of soil under fast-changing temperatures was used to compare the temperature sensitivity(Q10)of SOC decomposition across land uses.Important Findings After 15-20 years of afforestation on paddy fields,SOC concentra-tion only slightly increased at the depth of 0--5 cm but decreased in deeper layers,which resulted in a net loss of SOC stock in the top 40cm.Seasonal increase of sOC was observed during the rice-growing period in croplands but not in afforested soils,suggest-ing a stronger SOC sequestration by paddy rice cropping.However,SOC sequestered under cropping was more labile,as indicated by its higher contents of dissolved organic carbon and microbial bio-mass.Also,paddy soils had higher annual R,than afforested soils;R,abruptly increased after paddy fields were drained and plowed and remained distinctively high throughout the dry farming period.Laboratory incubation revealed that paddy soils had a much higher Q10 of SOC decomposition than afforested soils.Given that tem-perature was the primary controller of R,in this region,it was con-cluded that despite the stronger SOC sequestration by paddy rice cropping,its SOC was less stable than in afforested systems and might be more easily released into the atmosphere under global warming.

Salivary microbiota may predict the presence of esophageal squamous cell carcinoma

The aim is to explore the predictive value of salivary bacteria for the presence of esophageal squamous cell carcinoma (ESCC). Saliva samples were obtained from 178 patients with ESCC and 101 healthy controls, and allocated to screening and verification cohorts, respectively. In the screening phase, after saliva DNA was extracted, 16S rRNA V4 regions of salivary bacteria were amplified by polymerase chain reaction (PCR) with high-throughput sequencing. Highly expressed target bacteria were screened by Operational Taxonomic Units clustering, species annotation and microbial diversity assessment. In the verification phase, the expression levels of target bacteria identified in the screening phase were verified by absolute quantitative PCR (Q-PCR). Receiver operating characteristic (ROC) curves were plotted to investigate the predictive value of target salivary bacteria. LEfSe analysis revealed higher proportions of Fusobacterium, Streptococcus and Porphyromonas, and Q-PCR assay showed significantly higher numbers of Streptococcus salivarius, Fusobacterium nucleatum and Porphyromonas gingivalis in patients with ESCC, when compared with healthy controls (all P < 0.05). The areas under the ROC curves for Streptococcus salivarius, Fusobacterium nucleatum, Porphyromonas gingivalis and the combination of the three bacteria for predicting patients with ESCC were 69%, 56.5%, 61.8% and 76.4%, respectively. The sensitivities corresponding to cutoff value were 69.3%, 22.7%, 35.2% and 86.4%, respectively, and the matched specificity were 78.4%, 96.1%, 90.2% and 58.8%, respectively. These highly expressed Streptococcus salivarius, Fusobacterium nucleatum and Porphyromonas gingivalis in the saliva, alone or in combination, indicate their predictive value for ESCC.

Enhanced ionic diffusion interface in hierarchical metal-organic framework@layered double hydroxide for high-performance hybrid supercapacitors

Layered double hydroxides(LDHs)with abundant accessible active sites are promising electrode materials for hybrid supercapacitor(HSC)due to their ultrahigh theoretical capacitances.However,the structural agglomeration of LDH leads to poor rate capability and durability.Herein,we construct a diffusion-controlled interface in hierarchical architecture of metal-organic framework(MOF)HKUST-1@cobalt-nickel LDH(denoted as HKUST-1@CoNiLDH)through an in situ etching/electro-deposition strategy.The rapid charge transfer and ionic diffusion in HKUST-1@CoNiLDH deliver a remarkable specific capacity of 297.23 mAh·g^(−1) at 1 A·g^(−1),superior to mostly reported LDH-based electrodes.More importantly,the as-prepared HKUST-1@CoNiLDH//activated carbon HSC exhibit a high energy density of 39.8 Wh·kg^(−1) at a power density of 799.9 W·kg^(−1) with an outstanding capacitance retention of 90%after 5,000 charge–discharge cycles.The in-depth understanding of the ionic diffusion among the MOF/LDH interfaces will greatly promote the further development of designing and synthesizing high performance energy conversion and storage devices.

Surface decorated Ni sites for superior photocatalytic hydrogen production

Precise construction of isolated reactive centers on semiconductors with well-controlled configurations affords a great opportunity to investigate the reaction mechanisms in the photocatalytic process and realize the targeted conversion of solar energy to steer the charge kinetics for hydrogen evolution.In the current research,we decorated isolated Ni atoms on the surface of CdS nanowires for efficient photocatalytic hydrogen production.X-ray absorption fine structure investigations clearly demonstrate the atomical dispersion of Ni sites on the surface of CdS nanowires.Experimental investigations reveal that the isolated Ni atoms not only perform well as the real reactive centers but also greatly accelerate the electron transfer via direct Ni-S coordination.Theoretical simulation further documents that the hydrogen adsorption process has also been enhanced over the semi-coordinated Ni centers through electronic coupling at the atomic scale.

超声报告模板使用现状的问卷调查分析

目的调查分析我国超声报告模板使用现状及超声医师相关需求。方法以我国不同省市自治区直辖市的各级医院的超声医师为调查对象,采用互联网线上方式对超声报告模板使用现状,高效、规范化超声报告模板的主观需求程度进行调查分析。采用R×C列联表χ2检验,比较分析不同级别医院超声医师反馈之间的差异。结果本调查共收回有效答卷3863份,除香港特别行政区、澳门特别行政区及台湾省之外的全国31个省级行政区均有超声医师响应了此次问卷调查。问卷应答率方面:在地理分布、医院级别、职称类型方面均有一定差异,其中华北地区、三级医院、主治医师应答率最高,分别为30.44%(1176/3863)、53.46%(2065/3863)和41.11%(1588/3863)。无超声工作站和有超声工作站但无报告模板者共96份(2.49%,96/3863)答卷,有超声工作站并有报告模板者3767份(97.51%,3767/3863)答卷。在超声报告模板使用高效性方面:43.40%(1635/3767)的超声医师反馈需要用鼠标或键盘操作≥4步才能调出报告模板;93.05%(3505/3767)的超声医师表示,在遇到阳性病例时,“经常需要”或“一般需要”在报告模板的基础上修改较多文字;对于常见病是否都有超声报告模板的调查,“几乎全部常见病都有模板”者仅占37.09%(1397/3767),而常见病的不同严重程度是否有相应的报告模板方面,仅35.07%(1321/3767)的超声医师反馈有。在超声报告模板规范化方面:对于报告模板内容描述是否全面的调查,仅16.11%(607/3767)的超声医师认为所在科室报告模板内容描述“非常全面”;以甲状腺结节分级诊断(甲状腺超声影像报告和数据系统)所描述内容为标准,仅22.40%(832/3715)的超声医师反馈每一份甲状腺结节报告均描述全面;针对报告模板术语是否规范的调查,仅13.75%(518/3767)的超声医师认为所在科室报告模板术语使用“非常规范”,56.78%(2139/3767)的超声医师反馈所在科室超声报告模板中有“光点”“光团”等文字。对高效、规范化超声报告模板的主观需求方面:98.52%(3806/3863)的超声医师反馈需要一套使用高效、内容规范的超声报告模板。不同级别医院超声医师对所有上述几方面调查问题的答复,差异均具有统计学意义(P均<0.01),三级医院的超声报告模板在高效性及规范程度方面优于其他级别医院。结论目前我国超声报告模板在使用高效性及规范化程度方面均存在一定的不足,多数超声医师希望有一套使用高效的规范化超声报告模板。

Kinetically accelerated and high-mass loaded lithium storage enabled by atomic iron embedded carbon nanofibers

Carbonaceous materials represent the dominant choice of materials for anodic lithium storage in many energy storage devices.Nevertheless,the nonpolar carbonaceous materials offer weak adsorption toward Li+that largely denies the high-rate Li+storage.Herein,the atomic Fe sites decorated carbon nanofibers(AICNFs)facilely produced by electrospinning are reported for kinetically accelerated Li+storage.Theoretical calculation reveals that the atomic Fe sites possess coordination unsaturated electronic configuration,enabling suitable bonding energy and facilitated diffusion path of Li+.As a result,the optimal structure displays a high capacitive contribution up to 95.9%at a scan rate of 2.0 mV·s^(−1).In addition,ultrahigh capacity retention of 97%is afforded after 5,000 cycles at a current density of 3 A·g^(−1).Moreover,the interlaced fiber structure enabled by electrospinning benefits structural stability and improved conductivity even at thick electrodes,thus allowing a high areal capacity of 1.76 mAh·cm−2 at a loading of 8 mg·cm−2.Because of these structure and performance merits,the lithium-ion capacitor containing the AICNF-based anode delivers a high energy density and large power density.