Performance enhancement and active sites identification of Cu-Cd bimetallic oxide derived catalysts for electrochemical CO_(2) reduction

The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of challenge.Here,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 h.Interestingly,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such catalysts.The results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.

In-situ constructing Cu_(1)Bi_(1)bimetallic catalyst to promote the electroreduction of CO_(2)to formate by synergistic electronic and geometric effects

Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.

Controllably partial removal of thiolate ligands from unsupported Au_(25) nanoclusters by rapid thermal treatments for electrochemical CO_(2)reduction

Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core structure.This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of duration.This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction.Consequently,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be promoted.This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.

Hsa_circ_0036740 in familial adenomatous polyposis:Immune regulation and neutrophil effects in CRC based on highthroughput assay

Familial adenomatous polyposis(FAP)is an autosomal dominant disease with a high probability of becoming cancerous.Many RNAs potentially associated with FAP have not been identified.In this study,a circRNA(circular RNA)expression profile of FAP was established using a circRNA microarray,and differentially expressed circRNAs were verified by RT-qPCR.The effects of hsa_circ_0036740 on the malignant behavior of tumor cells(proliferation,apoptosis,and epithelial mesenchymal transition)and the levels of C3A complement protein expression were evaluated.Moreover,neutrophils were isolated and co-cultured with colorectal cancer cells(CRCs),followed by measurements of MPO-DNA,citrullinated histone H3,interleukin(IL)-1β,IL-6,and IL-8 levels.Nuclear translocation of arginine deiminase 4(PAD4)was observed using immunofluorescence assays.Based on the high-throughput assay,238 downregulated circRNAs,and 38 upregulated circRNAs were identified.A Kyoto Encyclopedia of Genes and Genomes enrichment analysis suggested that immune regulation might be involved in FAP.A total of 10 DECs(differentially expressed circular RNAs)were identified by RT-qPCR,and among them,hsa_circ_0036740 showed the highest fold-change in upregulation.Results of gain-of-and loss-of-function studies revealed that hsa_circ_0036740 enhanced the malignant behavior of tumor cells,such as metastasis,proliferation,and apoptosis,with an increasing level of C3A complement.Moreover,hsa_circ_0036740 also significantly increased neutrophil extracellular trap formation and inflammation in neutrophils,as shown by an increased expression of PAD4.In conclusion,this study revealed the expression profiles of circRNAs in FAP and confirmed the possible involvement of hsa_circ_0036740 in the immune regulation mediated by neutrophils.Finally,hsa_circ_0036740 was suggested as a new therapeutic target for CRC.

Progress and Challenges Toward Effective Flexible Perovskite Solar Cells

The demand for building-integrated photovoltaics and portable energy systems based on flexible photovoltaic technology such as perovskite embedded with exceptional flexibility and a superior power-to-mass ratio is enormous.The photoactive layer,i.e.,the perovskite thin film,as a critical component of flexible perovskite solar cells(F-PSCs),still faces long-term stability issues when deformation occurs due to encountering temperature changes that also affect intrinsic rigidity.This literature investigation summarizes the main factors responsible for the rapid destruction of F-PSCs.We focus on long-term mechanical stability of F-PSCs together with the recent research protocols for improving this performance.Furthermore,we specify the progress in F-PSCs concerning precise design strategies of the functional layer to enhance the flexural endurance of perovskite films,such as internal stress engineering,grain boundary modification,self-healing strategy,and crystallization regulation.The existing challenges of oxygen-moisture stability and advanced encapsulation technologies of F-PSCs are also discussed.As concluding remarks,we propose our viewpoints on the large-scale commercial application of F-PSCs.

Effects of Maize Silage Harvest Stage on Growth Performance and Economic Benefits of Beef Cattle

[Objectives]This study aimed to investigate the effects of whole-crop maize silage harvested at different stages on growth and economic benefits of beef cattle.[Methods]A total of 30 Simmental crossbred cattle weighing about 378 kg were randomly divided into three groups,respectively fed for 70 days with whole-crop maize silage harvested at milk stage(GroupⅠ),dough stage(GroupⅡ)and physiological maturity stage(GroupⅢ).Moreover,the cattle in all groups were given the same concentrate diet.[Results]There were significant differences in dry matter,crude protein and neutral detergent fiber between whole-crop maize silages harvested at different stages(P<0.05).The dry matter in GroupⅡandⅢwas significantly higher than that in GroupⅠ(P<0.05).The crude protein content peaked in GroupⅡ,up to 6.37%,which was significantly higher than that in GroupⅠ(by 12.74%,P<0.05)and GroupⅢ(by 9.26%,P<0.05).Starch content significantly increased with the postponing of maize harvest(P<0.05).The content of neutral detergent fiber in Group I was significantly higher than that in GroupⅡ(P<0.05)and GroupⅢ(P<0.05).The average daily weight gain in GroupⅡwas 8.53%higher than that in GroupⅠ(P<0.05)and 3.70%higher than that in GroupⅢ(P>0.05).The dry matter intake in GroupⅡwas significantly higher than that in GroupⅠ(P<0.05)and GroupⅢ(P<0.05).There was no significant difference in feed/gain ratio between the groups(P>0.05).The economic benefit in GroupⅡwas the highest,up to 9.99 yuan/day per capita.,followed by that in GroupⅢ,9.79 yuan/day per capita,and that in GroupⅠwas the lowest,only 8.03 yuan/day per capita.[Conclusions]The whole-crop maize silage harvested at dough stage has the best quality and produces the highest economic returns for beef cattle.

Effects of Whole-plant Corn Silage and Whole-plant Wheat Silage on Growth Performance and Economic Benefits of Beef Cattle

[Objectives]This study was conducted to study the effects of whole-plant corn silage and whole-plant wheat silage on growth performance and economic benefits of beef cattle.[Methods]Thirty Simmental crossbred cattle were selected and randomly divided based on their weight into two groups,15 cows in each group,with an average weight of 398 kg.Each group was fed the same concentrated feed,and the whole-plant corn silage and wheat silage were fed as roughage feed,respectively.The experimental period was 90 d.[Results](1)There was no significant difference in the initial weight of beef cattle between test group 1 and test group 2(P>0.05).Compared with group 2,group 1 had a higher final weight,average daily gain,and dry matter intake of beef cattle,without significant differences(P>0.05).Group 1 was 0.58%,1.99%,and 1.43%higher than group 2,respectively.The feed-to-gain ratio of test group 1 decreased by 0.54%compared with test group 2(P>0.05),with no significant difference therebetween.(2)The economic benefit of group 1 was 11.45 yuan/(day·capita),while the economic benefit of group 2 was 2.41 yuan/(day·capita),and group 1 was 9.04 yuan/(day·capita)higher than group 2.[Conclusions]Whole-plant corn silage for feeding beef cattle has the advantages of good weight gain and low breeding cost,and can be popularized in beef cattle fattening.

Multiple Pesticide Residues in Bananas Sold in Tangshan City and Dietary Risk Assessment

[Objectives]This study was conducted to investigate the pesticide residue status of bananas in Tangshan area and the dietary intake risk of consumers.[Methods]High-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS)was applied to detect 70 pesticide residues in 191 batches of banana samples extracted from Tangshan area,and chronic and acute risk assessments were conducted.[Results]Among the 191 batches of bananas,172 batches of samples were detected to contain agrochemicals,with a detection rate of 90.05%.Seventeen agrochemicals were detected,accounting for 24.29%of the total agrochemicals tested.There was a phenomenon of multiple pesticide residues in a single sample,and high detection rates were found in carbendazim(49.21%),prochloraz(41.88%),pyraclostrobin(34.03%)and imidacloprid(30.37%).According to GB 2763-2021 National Food Safety Standards—Maximum Residue Limits for Pesticides in Food,the over-standard rate of imidacloprid was 17.8%;and the chronic and acute dietary risks of the 17 pesticide residues were all less than 100%.[Conclusions]The pesticide residues in bananas consumed by consumers on a daily basis do not pose unacceptable dietary risks.

Nature of active phase of VO_x catalysts supported on SiBeta for direct dehydrogenation of propane to propylene

The VOx catalysts supported on dealuminated Beta zeolite(Si Beta) with varying V loadings(from 0.5 to 10 wt%) are prepared and tested for their catalytic activities in the reaction of direct dehydrogenation of propane to propylene(PDH). It is characterized that the VSi Beta catalysts possess different kinds of vanadium species on the Si Beta support, including monomeric or isolated VOx species at a low V loading, and polynuclear VOx species in different polymerization degrees at higher V loadings. The 3 VSi Beta catalyst(V loading is 3 wt%), containing isolated VOx species in monolayer, shows around 40% of propane conversion with 90% of propylene selectivity(reaction conditions: 600 o C, 4000 m L g–1 h–1) which are comparable to VSi Beta catalysts with higher V loadings. The catalytic activity exhibits a good linear relationship with the amount of generated acidic sites, which are derived from the interaction sites between VOx species and Si Beta support, and keeps stable after several regeneration cycles. Thus, as the VOx species directly contact with Si Beta support via V–O–Si bonds, a reactivity enhancement can be achieved. While, the initial valence state of V does not seem to influence the catalytic performance. Moreover, the aggregation degree of VOx species determines the propylene selectivity and deactivation rate, both of which increase as raising the V loading amount.

Integrated Ni2P nanosheet arrays on three-dimensional Ni foam for highly efficient water reduction and oxidation

The large-scale synthesis of efficient nonprecious bifunctional electrocatalysts for overall water splitting is a great challenge for future renewable energy conversion systems. Herein, Ni2P nanosheet arrays directly grown on three-dimensional(3 D) Ni foam(Ni P/NF) are fabricated by hydrothermal treatment of metallic Ni foam with H2O2solution and subsequent phosphidation with NaH2PO2. The Ni P/NF as electrocatalyst exhibits superior activities for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER). Most importantly, employing both as the cathode and anode for an alkaline water electrolyzer, Ni P/NF only requires a cell voltage of 1.63 V to reach a current density of 10 mV cm-2, together with stronger durability. Preliminary catalytic information suggests that the tailored 3 D superstructure and integrated electrode configurations afford improved active sties and enhanced electron/mass transfer,responding for the outstanding activity and stability.

Aluminum and phosphorus codoped “superaerophobic” Co3O4 microspheres for highly efficient electrochemical water splitting and Zn-air batteries

Multifunctional non-precious catalysts for hydrogen/oxygen evolution reaction(HER/OER) and oxygen reduction reaction(ORR) constitute the bottleneck in the applications in electrochemical overall water splitting(OWS) and Zn-air batteries. Herein, a trifunctional electrocatalyst of urchin-like Al,P-codoped Co3O4 microspheres supported on Ni foam(denoted as AP-CONPs/NF) was fabricated via a hydrothermal process and subsequent low-temperature annealing and phosphorization, exhibiting enhanced OER, HER and ORR activities compared with single-doped and undoped samples. Their surface self-organized microstructure and excellent "superaerophobic" feature make a high bubble repellency, which boost diffusion of reactants and electrolyte-electrode intimate contact. The codoping of Al and P elements into Co3O4 betters right the balance among surface chemical state, the increased oxygen vacancies and the promoted charge transfer. Encouraged by these synergistic advantages, the AP-CONPs/NF was further employed as excellent bifunctional electrodes for the OWS(low cell voltage of 1.57 V at 10 mA cm-2) and as air cathode for rechargeable Zn-air batteries(high power density of 89.1 mW cm-2), which demonstrates a great feasibility for practical applications.

A photo-assisted electrochemical-based demonstrator for green ammonia synthesis

Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been proposed for green ammonia synthesis from renewable electricity, air and water, where well-known defect-laden WO_(3) is used as the working electrode, and a commercially available PV panel supplies renewable electricity. In this demonstrator, defect-laden WO_(3) exhibits the optimum electrochemical NH_(3) formation rate(4.51 × 10^(-12)mol s^(-1)cm^(-2)) in 0.1 M K_(2)SO_(4)in a photovoltaic electrochemical(PV-EC) system. A system-level energy and cost analysis was conducted to investigate its economic viability and a general evaluation tool for system performance and cost estimation was proposed. This advance enables the possibility of integrating the small-scale green ammonia demonstrator into a stand-alone farm system.

Chemical Constituents of Pedicularis longiflora var. tubiformis (Orobanchaceae), a Common Hemiparasitic Medicinal Herb from the Qinghai Lake Basin, China

Pedicularis longiflora var.tubiformis(Orobanchaceae)is an abundant parasitic herb mainly found in the Xiaopohu wetland of the Qinghai Lake Basin in Northwestern China.The species has an important local medicinal value,and in this study,we evaluated the chemical profile of its stems,leaves and seeds using mass spectrometry.Dried samples of stems,leaves and seeds were grinded,weighted,and used for a series of extractions with an ultrasonic device at room temperature.The chemical profiles for each tissue were determined using Gas Chromatography-Mass Spectrometry(GC-MS)and Liquid Chromatography-Mass Spectrometry(LC-MS).Twenty-seven amino acids and organic acids were identified and quantified from stems,leaves and seeds.The content of amino acids detected in leaves and seeds was higher than the amount found in stems.Six fla-vonoids were also detected,including isoorientin,orientin,luteolin-7-O-glucoside,luteolin,apigenin and tricin.The concentrations of luteolin-7-O-glucoside,luteolin and tricin were the highest and more concentrated in leaves,while that of orientin was the lowest and mainly found in stems.Soluble monosaccharides and oligosaccharides below tetramer were also examined,and our analyses detected the presence of arabitol,fructose,galacturonic acid,glucose,glucuronic acid,inositol,sucrose,and trehalose.This is the first study to identify and quantify the main components of amino acids,organic acids,flavonoids and soluble sugars from stems,leaves and seeds of P.longiflora var.tubiformis.Eight of the amino acids detected are essential for humans,highlighting the medicinal importance of this species.Results shown here can be used as a reference case to develop future studies on the chemical constituents of Pedicularis herbs and other medicinal plants from the Tibetan region.

Wheat Elongator subunit 4 is required for epigenetic regulation of host immune response to Rhizoctonia cerealis

Wheat(Triticum aestivum)is necessary for global food security.The necrotrophic fungus Rhizoctonia cerealis is the causal agent of sharp eyespot,a devastating disease of wheat.Although the Elongator complex,composed of six subunits,has been implicated in growth,development,and innate immunity in Arabidopsis,little is known about its functions in wheat or the involvement of Elongator subunit 4 in histone acetylation.In this study,we identified the Elongator subunit 4-encoding gene Ta ELP4 in wheat resistance response to R.cerealis,and verified that Ta ELP4 increased histone acetylation in regions of defenseassociated genes and regulated immune response to R.cerealis.Ta ELP4 was more highly expressed in resistant than in susceptible wheat cultivars and was induced in resistant wheat after infection by R.cerealis.Silencing of Ta ELP4 in wheat not only impaired resistance to R.cerealis,but also repressed both histone acetylation levels and the expression of a subset of defense-associated genes,including Ta AGC1,Ta CPK7-D,Ta PAL5,Defensin,and Chitinase2.Ectopic expression of Ta ELP4 in Arabidopsis increased histone acetylation levels in coding and promoter regions of defense genes and increased their transcription,leading to increased resistance to infection by the pathogen Botrytis cinerea.These results suggest that Ta ELP4 positively regulates innate immune responses of wheat and Arabidopsis to R.cerealis and B.cinerea by increasing histone acetylation levels of defense-associated genes and increasing their transcription.This study has shed light on the involvement of Ta ELP4 in histone acetylation and resistance response against R.cerealis.Ta ELP4 may potentially be used to improve wheat resistance against sharp eyespot.

Five Point Methodology of XRD Second Derivative Fingerprint to Meconopsis

In the paper, using the method of Lagrange interpolation five formulas, the second derivative written is obtained from XRD （X-ray diffraction） spectrum graph of MATLAB. Methodology of XRD SD （X-ray diffraction second derivative） was adapted to extract low frequency signal from original XRD patterns of traditional Chinese medicine. The results indicated that the XRD SD fingerprints obtained had obvious peak with sharp profile, which could distinctly embody the digital characteristics of different Meconopsis. Otherwise, the results also showed that XRD SD fingerprints might be a promising method for identification and quantity control for traditional Chinese medicine and could effectively solve the problem of XRD spectrum analytical dispersion type plant medicine and had a function of magnifying glass.

Study on the clinical application of pain treatment efficacy evaluation and the nursing of patients with chronic noncancer pain

Objective:To evaluate the pain degree of the patients with chronic non-cancer pain by using the evaluation model constituted by heart rate variability,anxiety and depression scale and quality of life rating scale,and to evaluate the efficacy after treatment and nursing intervention.Methods:100 patients with chronic non-cancer pain treated in our hospital from February 2016 to April 2017 were selected to compare their heart rate variability,score of anxiety and depression,score of quality of life and NRS score before and after treatment and nursing intervention.Results:After treatment and nursing intervention,the heart rate variability time domain SDNN increased and the difference is significant(P<0.05);the score of anxiety and depression was lower than that before intervention(P<0.05);the scores of various dimensions of quality of life were higher than those before intervention(P<0.05);the NRS score was lower than that before intervention(P<0.05).Conclusion:The evaluation model constituted by heart rate variability,anxiety and depression scale and quality of life rating scale can be used to evaluate the pain degree of the patients with chronic non-cancer pain and to evaluate the efficacy after treatment and nursing intervention,which is worthy of clinic application.

环境信息披露对企业可持续发展能力的影响研究——来自于重污染行业的经验数据

本文选取2012—2021年A股上市公司重污染行业的企业作为研究对象,对环境信息披露质量对于企业可持续发展能力的作用关系进行实证分析。研究发现:环境信息披露对企业可持续发展能力具有显著的正向影响,高质量的环境信息披露会促进企业可持续发展。市场竞争程度可以降低环境信息披露对企业可持续发展能力的促进作用,企业所处的市场环境竞争程度越大,环境信息披露对企业可持续发展能力的影响越小。重污染企业环境信息披露对企业可持续发展能力的提升效应在非国有企业和高竞争度的市场环境中更为明显。本文的研究结论有助于深入理解环境信息披露和企业可持续发展能力之间的关系,为如何提升企业可持续发展能力提出了新的角度与思路。

环境条件下电催化氮还原的现状、挑战与展望

氨是一种重要的化肥生产原料和清洁能源载体,在工业上主要通过哈伯法合成,但该工艺反应条件苛刻,需要高温高压并消耗大量的化石能源。因此,开发能耗低、反应温和的合成氨方法,对于缓解能源和环境的双重压力具有重要的现实意义。近年来,在温和条件下通过电催化氮还原反应(NRR)合成氨有望替代哈伯法,但该技术的重点在于设计合理的电催化反应体系并开发高效的催化剂以提升缓慢的NRR动力学过程。为此,本文从电催化合成氨的反应机理出发,介绍了电催化氮还原体系的构建,综述了近年来电催化氮还原催化剂的发展现状,重点总结了提升NRR催化剂活性的设计策略,并对这一新兴领域面临的挑战和潜在的应用前景进行了合理的展望。

自支撑型过渡金属磷化物电催化析氢反应研究

氢能作为一种零碳排放的清洁能源,主要通过电解水的途径获得。电解水析氢过程所使用的贵金属Pt基催化剂非常稀缺和昂贵,因此开发具有高活性和稳定性的非贵金属催化剂仍然是一个巨大的挑战。自支撑型过渡金属磷化物析氢性能优异,加之有效结合了自支撑基底的诸多优势,有望成为可替代贵金属Pt基催化剂的优良析氢材料。本文详细介绍了自支撑型过渡金属磷化物的研究进展,着重论述了此类型电催化剂的析氢优势及作用机理:(1)自支撑基底3D集成框架导电性较强,可提供大量的电子转移通道,从而加速催化反应进程;(2)自支撑型过渡金属磷化物较大的比表面积将会暴露出更多的活性位点,进而促进催化反应的发生;(3)自支撑型过渡金属磷化物可以直接作为阴极进行析氢反应,避免传统涂覆法中催化剂容易从玻碳电极脱落的弊端。最后,总结了此类型电催化剂用于电解水反应所面临的问题和挑战,并进行了合理的展望。

Detection of serum IgM and IgG for COVID-19 diagnosis

Dear Editor,Infection with the novel coronavirus(SARS-CoV-2,which is the virus responsible for the coronavirus disease 2019(COVID-19))was first reported in Wuhan,China on December 31,2019.The outbreak of COVID-19 remains ongoing and was linked to more than 80,000 infected patients and more than 3,000 deaths in China as of March 7,2020(Holshue et al.,2020).