Pub Date : 2025-01-01Epub Date: 2024-10-15DOI: 10.1016/j.talanta.2024.127049
Zhenjie Qiao, Shuzhen Yue, Xiaoyue Zhang, Pengfei Shi, Shuzhen Lv, Sai Bi
The controllable geometry and multifunctionality of DNA nano-bioreactors hold immense promise for disease diagnosis. Herein, a facile rolling circle amplification (RCA)-based crystallization method has been developed for highly efficient self-assembly of three-dimensional (3D) DNA nano-bioreactors, which show excellent cascade catalytic performance by confining bio-enzyme (glucose oxidase (GOx) used in this case) and copper ions (Cu2+) in DNA nanoflowers (DNFs) structure. The participation of Cu2+ during the self-assembly process not only endows the nano-bioreactors (designated as GOx/Cu@DNFs) with inspiring peroxidase-like activity but also greatly improves the assembly efficiency and yield via the effective coordination between Cu2+ and RCA-generated long concatemeric DNAs. The integration of GOx and Cu2+ in the constrained flower-like DNA nanomatrices makes for the efficient inter-catalyst communication, resulting in the striking enhancement of biocatalytic cascade activity. Based on the prepared nano-bioreactors, a colorimetric biosensor has been constructed for glucose detection, achieving a wide linear range (2-400 μM) and a low detection limit (0.45 μM). Furthermore, the proposed sensing strategy enables the accurate determination and discrimination of glucose levels in healthy and diabetic sera, delivering gratifying outcomes. Overall, the meticulously crafted cascade nano-bioreactors not only illuminate the design of multifunctional nanomaterials based on RCA, but also expand the conceptual framework of the universal analytical method for determining small molecules with catalytic reactions to generate H2O2.
DNA 纳米生物反应器的可控几何形状和多功能性为疾病诊断带来了巨大前景。在此,我们开发了一种基于滚圆放大(RCA)的简便结晶方法,用于高效自组装三维(3D)DNA 纳米生物反应器,这种反应器通过将生物酶(本例中使用的是葡萄糖氧化酶(GOx))和铜离子(Cu2+)限制在 DNA 纳米花(DNFs)结构中,显示出卓越的级联催化性能。Cu2+ 在自组装过程中的参与不仅赋予了纳米生物反应器(命名为 GOx/Cu@DNFs)鼓舞人心的过氧化物酶样活性,而且通过 Cu2+ 与 RCA 生成的长连接 DNA 之间的有效配位,大大提高了组装效率和产量。GOx 和 Cu2+ 在受约束的花朵状 DNA 纳米结构中的整合使得催化剂之间可以进行有效的交流,从而显著提高了生物催化级联活性。基于制备的纳米生物反应器,构建了一种用于葡萄糖检测的比色生物传感器,实现了宽线性范围(2-400 μM)和低检测限(0.45 μM)。此外,所提出的传感策略还能准确测定和区分健康血清和糖尿病血清中的葡萄糖水平,结果令人满意。总之,精心制作的级联纳米生物反应器不仅阐明了基于 RCA 的多功能纳米材料的设计,还拓展了利用催化反应生成 H2O2 来测定小分子的通用分析方法的概念框架。
{"title":"Copper ions coordination-promoted self-assembly of DNA nanoflowers as cascade catalytic nanoreactor for colorimetric biosensor.","authors":"Zhenjie Qiao, Shuzhen Yue, Xiaoyue Zhang, Pengfei Shi, Shuzhen Lv, Sai Bi","doi":"10.1016/j.talanta.2024.127049","DOIUrl":"10.1016/j.talanta.2024.127049","url":null,"abstract":"<p><p>The controllable geometry and multifunctionality of DNA nano-bioreactors hold immense promise for disease diagnosis. Herein, a facile rolling circle amplification (RCA)-based crystallization method has been developed for highly efficient self-assembly of three-dimensional (3D) DNA nano-bioreactors, which show excellent cascade catalytic performance by confining bio-enzyme (glucose oxidase (GOx) used in this case) and copper ions (Cu<sup>2+</sup>) in DNA nanoflowers (DNFs) structure. The participation of Cu<sup>2+</sup> during the self-assembly process not only endows the nano-bioreactors (designated as GOx/Cu@DNFs) with inspiring peroxidase-like activity but also greatly improves the assembly efficiency and yield via the effective coordination between Cu<sup>2+</sup> and RCA-generated long concatemeric DNAs. The integration of GOx and Cu<sup>2+</sup> in the constrained flower-like DNA nanomatrices makes for the efficient inter-catalyst communication, resulting in the striking enhancement of biocatalytic cascade activity. Based on the prepared nano-bioreactors, a colorimetric biosensor has been constructed for glucose detection, achieving a wide linear range (2-400 μM) and a low detection limit (0.45 μM). Furthermore, the proposed sensing strategy enables the accurate determination and discrimination of glucose levels in healthy and diabetic sera, delivering gratifying outcomes. Overall, the meticulously crafted cascade nano-bioreactors not only illuminate the design of multifunctional nanomaterials based on RCA, but also expand the conceptual framework of the universal analytical method for determining small molecules with catalytic reactions to generate H<sub>2</sub>O<sub>2</sub>.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127049"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
It is essential to develop a multifunctional nanoplatform for biosensing, tumor diagnosis and treatment simultaneously. Herein, dual-emission fluorescent carbon dots (HA-CDs) were fabricated via a one-pot solvothermal method using spinach powder as carbon source and hyaluronic acid (HA) as targeting agent. The obtained HA-CDs exhibited outstanding optical properties, good targeted tumor and excellent photothermal conversion performance. Interestingly, HA-CDs can sensitively perceive the changes in polar environments attributed to the inherent ratiometric fluorescence characteristics, and combined with the intrinsic targeting tumor ability achieved tumor cell recognition. More importantly, the HA-CDs possess good photothermal conversion efficiency of 21.2 % to be beneficial for photothermal therapy of tumors. The survival rate of HeLa cells incubated with HA-CDs dramatically decreased to 14 % after 660 nm laser irradiation, revealing the significant tumor inhibition of HA-CDs in vitro. Notably, through individual intraperitoneal and intratumoral injection, it was found that HA-CDs demonstrated a similar tumor suppressed effect on 4T1 tumor-bearing mice exposed to laser irradiation, fully uncovering that HA-CDs can efficiently accumulate at tumor site by intraperitoneal injection. Besides, the histopathological analysis of major organs ex vivo revealed a good biosafety profile. Collectively, this strategy of designed HA-CDs provides a new multifunctional nanoplatform for potential clinical application.
{"title":"Dual-emission carbon dots-based biosensor for polarity/targeting bimodal recognition and mild photothermal therapy of tumor.","authors":"Xiaorui Dong, Wenjun Yan, Dongmei Zhang, Ruihan Wang, Liuyan Xue, Heping Shi, Yingqi Li","doi":"10.1016/j.talanta.2024.127060","DOIUrl":"10.1016/j.talanta.2024.127060","url":null,"abstract":"<p><p>It is essential to develop a multifunctional nanoplatform for biosensing, tumor diagnosis and treatment simultaneously. Herein, dual-emission fluorescent carbon dots (HA-CDs) were fabricated via a one-pot solvothermal method using spinach powder as carbon source and hyaluronic acid (HA) as targeting agent. The obtained HA-CDs exhibited outstanding optical properties, good targeted tumor and excellent photothermal conversion performance. Interestingly, HA-CDs can sensitively perceive the changes in polar environments attributed to the inherent ratiometric fluorescence characteristics, and combined with the intrinsic targeting tumor ability achieved tumor cell recognition. More importantly, the HA-CDs possess good photothermal conversion efficiency of 21.2 % to be beneficial for photothermal therapy of tumors. The survival rate of HeLa cells incubated with HA-CDs dramatically decreased to 14 % after 660 nm laser irradiation, revealing the significant tumor inhibition of HA-CDs in vitro. Notably, through individual intraperitoneal and intratumoral injection, it was found that HA-CDs demonstrated a similar tumor suppressed effect on 4T1 tumor-bearing mice exposed to laser irradiation, fully uncovering that HA-CDs can efficiently accumulate at tumor site by intraperitoneal injection. Besides, the histopathological analysis of major organs ex vivo revealed a good biosafety profile. Collectively, this strategy of designed HA-CDs provides a new multifunctional nanoplatform for potential clinical application.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127060"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
To overcome the limitations of insufficient sensitivity and poor specificity of portable screen-printed carbon electrode-electrochemical sensors (SPCE-EC) in practical applications, we prepared carrier composites of carboxylic single-walled carbon nanotubes vertically grafted by covalent organic frameworks (v-COF@SWCNTs-COOH) and coated with a molecularly imprinted polymer (MIP) of sulfadimidine (SM2). 55 °C hot steam elution is more eco-friendly than traditional organic solvent elution. The results showed that when the mass ratio of DBA to DBA-SWCNTs was 1:1, the v-COF@SWCNTs-COOH obtained by the two-step synthesis method could increase the electrical signal up to 2.33-fold of the bare electrode. The bifunctional monomer MIP prepared on the above structure enhanced the signal response by 2.91-fold, with a high imprint factor of 20. The assembled MIP/v-COF@SWCNTs-COOH/SPCE were analyzed by differential pulse voltammetry (DPV) with a high sensitivity of 0.21 nM for LOD and 0.70 nM for LOQ. In milk and fish samples, the recovery rate was 95.0 %-104.8 %. The validation of authentic pork samples with the statutory LC-MS/MS method showed no significant difference (P > 0.05). The sensor's performance indicators remained robust after five repeated uses. Therefore, the MIP/v-COF@SWCNTs-COOH/SPCE combines the cheapness and portability of SPCE, while the sensitivity and specificity of small molecule detection were significantly improved.
{"title":"Preparation of a V-COF@SWCNTs-COOH/SPCE supported molecularly imprinted electrochemical sensor for real-time detection of trace sulfadimidine.","authors":"Shuomeng Bai, Tingting Yang, Peiqiao Liu, Junhua Tan, Shuixie Chen, Hongtao Lei, Xiaoqun Wei","doi":"10.1016/j.talanta.2024.127046","DOIUrl":"10.1016/j.talanta.2024.127046","url":null,"abstract":"<p><p>To overcome the limitations of insufficient sensitivity and poor specificity of portable screen-printed carbon electrode-electrochemical sensors (SPCE-EC) in practical applications, we prepared carrier composites of carboxylic single-walled carbon nanotubes vertically grafted by covalent organic frameworks (v-COF@SWCNTs-COOH) and coated with a molecularly imprinted polymer (MIP) of sulfadimidine (SM<sub>2</sub>). 55 °C hot steam elution is more eco-friendly than traditional organic solvent elution. The results showed that when the mass ratio of DBA to DBA-SWCNTs was 1:1, the v-COF@SWCNTs-COOH obtained by the two-step synthesis method could increase the electrical signal up to 2.33-fold of the bare electrode. The bifunctional monomer MIP prepared on the above structure enhanced the signal response by 2.91-fold, with a high imprint factor of 20. The assembled MIP/v-COF@SWCNTs-COOH/SPCE were analyzed by differential pulse voltammetry (DPV) with a high sensitivity of 0.21 nM for LOD and 0.70 nM for LOQ. In milk and fish samples, the recovery rate was 95.0 %-104.8 %. The validation of authentic pork samples with the statutory LC-MS/MS method showed no significant difference (P > 0.05). The sensor's performance indicators remained robust after five repeated uses. Therefore, the MIP/v-COF@SWCNTs-COOH/SPCE combines the cheapness and portability of SPCE, while the sensitivity and specificity of small molecule detection were significantly improved.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127046"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-10-15DOI: 10.1016/j.talanta.2024.127054
Kai Zhang, Yule Qian, Chaoyan Lou, Mingli Ye, Yan Zhu
PyICLab is an open-source Python-based package featuring an object-oriented programming (OOP) interface, providing tools for realistic and customized numerical simulations of ion chromatography (IC). In this paper, we showcase PyICLab's use in simulating diverse separation scenarios, including isocratic carbonate elution, gradient hydroxide elution, high-concentration and large-volume injections. The accuracy of the embedded models was validated by demonstrating strong correlations between predicted and experimental results. Additionally, PyICLab's capability to handle complex IC configurations was demonstrated through a simulation of a column-switching system for seawater analysis. PyICLab offers valuable resources for chromatographic optimization, method development, and educational purposes. It is available on PyPI at pypi.org/project/pyIClab. Interested readers can install PyICLab using the pip command in a Python 3.11 or higher environment.
{"title":"PyICLab: An integrated Python-based toolkit for in-silico simulations of ion chromatography.","authors":"Kai Zhang, Yule Qian, Chaoyan Lou, Mingli Ye, Yan Zhu","doi":"10.1016/j.talanta.2024.127054","DOIUrl":"10.1016/j.talanta.2024.127054","url":null,"abstract":"<p><p>PyICLab is an open-source Python-based package featuring an object-oriented programming (OOP) interface, providing tools for realistic and customized numerical simulations of ion chromatography (IC). In this paper, we showcase PyICLab's use in simulating diverse separation scenarios, including isocratic carbonate elution, gradient hydroxide elution, high-concentration and large-volume injections. The accuracy of the embedded models was validated by demonstrating strong correlations between predicted and experimental results. Additionally, PyICLab's capability to handle complex IC configurations was demonstrated through a simulation of a column-switching system for seawater analysis. PyICLab offers valuable resources for chromatographic optimization, method development, and educational purposes. It is available on PyPI at pypi.org/project/pyIClab. Interested readers can install PyICLab using the pip command in a Python 3.11 or higher environment.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127054"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-03-28DOI: 10.1177/10731911241240626
M F Facon, S P J van Alphen, E Dierckx, G Rossi
As previous studies have shown that personality disorder (PD) assessment in older adults is often hampered because assessment tools are tailored toward younger adults, establishing the age-neutrality of novel tools is crucial. This study primarily aimed to evaluate the age-neutrality of the Level of Personality Functioning Brief Form (LPFS-BF 2.0) and the Personality Inventory for DSM-5 Modified + (PID-5-BF+M), using a sample of 254 community-dwelling adults. The analysis of Differential Item Functioning (DIF) demonstrated the age-neutrality of both instruments, with only 8.3% of LPFS-BF 2.0 items and 5.6% of PID-5-BF+M items exhibiting DIF. Differential Test Functioning (DTF) analyses revealed large DTF for the LPFS-BF 2.0 total score, indicating that age-specific norms might be necessary for this score. In summary, this study supports the use of these instruments in both older and younger adults, enhancing the assessment of PDs across the life span.
{"title":"Age-Neutral Measurement Of Personality Functioning and Maladaptive Personality Traits.","authors":"M F Facon, S P J van Alphen, E Dierckx, G Rossi","doi":"10.1177/10731911241240626","DOIUrl":"10.1177/10731911241240626","url":null,"abstract":"<p><p>As previous studies have shown that personality disorder (PD) assessment in older adults is often hampered because assessment tools are tailored toward younger adults, establishing the age-neutrality of novel tools is crucial. This study primarily aimed to evaluate the age-neutrality of the Level of Personality Functioning Brief Form (LPFS-BF 2.0) and the Personality Inventory for <i>DSM</i>-5 Modified + (PID-5-BF+M), using a sample of 254 community-dwelling adults. The analysis of Differential Item Functioning (DIF) demonstrated the age-neutrality of both instruments, with only 8.3% of LPFS-BF 2.0 items and 5.6% of PID-5-BF+M items exhibiting DIF. Differential Test Functioning (DTF) analyses revealed large DTF for the LPFS-BF 2.0 total score, indicating that age-specific norms might be necessary for this score. In summary, this study supports the use of these instruments in both older and younger adults, enhancing the assessment of PDs across the life span.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":" ","pages":"3-13"},"PeriodicalIF":4.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140317699","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-03-14DOI: 10.1177/10731911241236687
Justin E Karr, Agnes E White, Sharon E Leong, T K Logan
This study psychometrically evaluated the Neurobehavioral Symptom Inventory (NSI) among women survivors of intimate partner violence (IPV) and compared symptoms between women with no brain injury history (n = 93) and women with IPV-related brain injury history (n = 112). Women completed the NSI and questionnaires on traumatic brain injury (TBI), hypoxic-ischemic brain injury (HI-BI), and lifetime IPV history. A four-factor NSI model, including affective, somatosensory, cognitive, and vestibular factors, had the best fit (comparative fit index = 0.970, root mean square error of approximation = 0.064), with strong reliability for the total score (ω = .93) and subscale scores (ω range = .72-.89). In group comparisons, women with IPV-related brain injuries reported greater total, affective, and cognitive symptom severity after adjusting for age and education; however, no group differences were observed after adjusting for IPV severity. When examining lifetime number of brain injuries, HI-BI count was independently predictive of total, cognitive, and vestibular symptom severity after adjusting for age, education, and IPV severity; whereas TBI count did not independently predict any NSI scores after adjusting for these covariates. The NSI had acceptable psychometric properties for measuring neurobehavioral symptoms among women survivors of IPV. The association between HI-BI count and cognitive and vestibular symptoms may indicate the importance of studying repetitive nonfatal strangulation as an injury mechanism in this population.
{"title":"The Neurobehavioral Symptom Inventory: Psychometric Properties and Symptom Comparisons in Women With and Without Brain Injuries Due to Intimate Partner Violence.","authors":"Justin E Karr, Agnes E White, Sharon E Leong, T K Logan","doi":"10.1177/10731911241236687","DOIUrl":"10.1177/10731911241236687","url":null,"abstract":"<p><p>This study psychometrically evaluated the Neurobehavioral Symptom Inventory (NSI) among women survivors of intimate partner violence (IPV) and compared symptoms between women with no brain injury history (<i>n</i> = 93) and women with IPV-related brain injury history (<i>n</i> = 112). Women completed the NSI and questionnaires on traumatic brain injury (TBI), hypoxic-ischemic brain injury (HI-BI), and lifetime IPV history. A four-factor NSI model, including affective, somatosensory, cognitive, and vestibular factors, had the best fit (comparative fit index = 0.970, root mean square error of approximation = 0.064), with strong reliability for the total score (<i>ω</i> = .93) and subscale scores (<i>ω</i> range = .72-.89). In group comparisons, women with IPV-related brain injuries reported greater total, affective, and cognitive symptom severity after adjusting for age and education; however, no group differences were observed after adjusting for IPV severity. When examining lifetime number of brain injuries, HI-BI count was independently predictive of total, cognitive, and vestibular symptom severity after adjusting for age, education, and IPV severity; whereas TBI count did not independently predict any NSI scores after adjusting for these covariates. The NSI had acceptable psychometric properties for measuring neurobehavioral symptoms among women survivors of IPV. The association between HI-BI count and cognitive and vestibular symptoms may indicate the importance of studying repetitive nonfatal strangulation as an injury mechanism in this population.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":" ","pages":"102-118"},"PeriodicalIF":4.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140118677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-03-16DOI: 10.1177/10731911241236351
Hanif Akhtar, Kristof Kovacs
Although many fluid reasoning (Gf) tests have been developed, there is a lack of figural tests measuring its lower-order process factors simultaneously. The present article introduces the development of the Multidimensional Induction-Deduction Computerized Adaptive Test (MID-CAT) to measure two process factors of Gf. The MID-CAT is designed to provide an instrument that is flexible, efficient, and entirely free for non-commercial use. We created 530 items and administered them to a sample of N = 2,247. Items were fitted and calibrated using the Rasch model. The results indicate that the final item pool has a wide range of difficulties that could precisely measure a wide range of test-takers' abilities. A simulation study also indicates that MID-CAT provides greater measurement efficiency than separate-unidimensional CAT or fixed-item test. In the discussion, we provide perspectives on how the MID-CAT can be used for future research.
{"title":"Measuring Process Factors of Fluid Reasoning Using Multidimensional Computerized Adaptive Testing.","authors":"Hanif Akhtar, Kristof Kovacs","doi":"10.1177/10731911241236351","DOIUrl":"10.1177/10731911241236351","url":null,"abstract":"<p><p>Although many fluid reasoning (Gf) tests have been developed, there is a lack of figural tests measuring its lower-order process factors simultaneously. The present article introduces the development of the Multidimensional Induction-Deduction Computerized Adaptive Test (MID-CAT) to measure two process factors of Gf. The MID-CAT is designed to provide an instrument that is flexible, efficient, and entirely free for non-commercial use. We created 530 items and administered them to a sample of <i>N</i> = 2,247. Items were fitted and calibrated using the Rasch model. The results indicate that the final item pool has a wide range of difficulties that could precisely measure a wide range of test-takers' abilities. A simulation study also indicates that MID-CAT provides greater measurement efficiency than separate-unidimensional CAT or fixed-item test. In the discussion, we provide perspectives on how the MID-CAT can be used for future research.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":" ","pages":"32-47"},"PeriodicalIF":4.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140139840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A robust interface for coupling capillary electrophoresis (CE) to mass spectrometry (MS) was critical to maintain high separation efficiency of CE while achieving high sensitivity of MS. Current interfaces often suffer from problems such as reproducibility and ruggedness. For this purpose, a new polymetallic-coated sheathless interface was developed for the coupling of CE with MS. The electrical contact of the interface was achieved by etching one end of the fused silica capillary into a tapered tip using hydrofluoric acid (HF) solution, and then depositing a thin layer of chromium followed by a layer of platinum on it via physical vapor deposition technique. The performance of the new sheathless interface was systematically evaluated for the effect of flow rate and electrospray ionization (ESI) voltage on MS signal intensity, as well as the sample loading volume on CE separation efficiency and repeatability by using peptide standards and tryptic digest of bovine serum albumin (BSA). The interface was capable of generating stable electrospray even at ultra-low flow rate of 12.2 nL/min. In addition, the acid and alkali resistance of the polymetallic-coated emitter was tested by immersing it into 1 M HCL and 1 M NaOH solution, respectively. The results showed that polymetallic coating was still intact even after continuous immersion in the alkaline solution for 8 days (192 h) and a longer period in the acidic solution, indicating its excellent chemical stability. All the experimental results indicated that the sheathless interface fabricated by the new method in this study was robust and stable, making it promising for both sensitive and robust CE-MS sample analysis.
要保持毛细管电泳(CE)的高分离效率,同时实现质谱(MS)的高灵敏度,必须有一个强大的接口将毛细管电泳(CE)与质谱(MS)耦合起来。目前的接口往往存在可重复性和坚固性等问题。为此,我们开发了一种新型聚金属涂层无护套接口,用于 CE 与 MS 的耦合。使用氢氟酸(HF)溶液将熔融石英毛细管的一端蚀刻成锥形尖端,然后通过物理气相沉积技术在其上沉积一薄层铬和一薄层铂,从而实现接口的电接触。通过使用肽标准品和牛血清白蛋白(BSA)胰蛋白酶消化物,系统评估了流速和电喷雾离子化(ESI)电压对质谱信号强度的影响,以及样品装载量对 CE 分离效率和重复性的影响,从而确定了新型无鞘接口的性能。即使在 12.2 nL/min 的超低流速下,该界面也能产生稳定的电喷雾。此外,还将多金属涂层发射器分别浸入 1 M HCL 和 1 M NaOH 溶液中测试其耐酸碱性。结果表明,即使在碱性溶液中连续浸泡 8 天(192 小时)以及在酸性溶液中浸泡更长时间,多金属涂层仍然完好无损,这表明多金属涂层具有出色的化学稳定性。所有实验结果表明,本研究中采用新方法制作的无鞘界面坚固稳定,有望用于灵敏、稳健的 CE-MS 样品分析。
{"title":"A robust polymetallic-coated sheathless interface with high acid and alkali resistance for coupling capillary electrophoresis with mass spectrometry.","authors":"Xiaozhong Hu, Wenqing Gao, Rong Liu, Chen Tang, Huanming Wu, Jiancheng Yu, Yuheng Wang, Keqi Tang","doi":"10.1016/j.talanta.2024.127045","DOIUrl":"10.1016/j.talanta.2024.127045","url":null,"abstract":"<p><p>A robust interface for coupling capillary electrophoresis (CE) to mass spectrometry (MS) was critical to maintain high separation efficiency of CE while achieving high sensitivity of MS. Current interfaces often suffer from problems such as reproducibility and ruggedness. For this purpose, a new polymetallic-coated sheathless interface was developed for the coupling of CE with MS. The electrical contact of the interface was achieved by etching one end of the fused silica capillary into a tapered tip using hydrofluoric acid (HF) solution, and then depositing a thin layer of chromium followed by a layer of platinum on it via physical vapor deposition technique. The performance of the new sheathless interface was systematically evaluated for the effect of flow rate and electrospray ionization (ESI) voltage on MS signal intensity, as well as the sample loading volume on CE separation efficiency and repeatability by using peptide standards and tryptic digest of bovine serum albumin (BSA). The interface was capable of generating stable electrospray even at ultra-low flow rate of 12.2 nL/min. In addition, the acid and alkali resistance of the polymetallic-coated emitter was tested by immersing it into 1 M HCL and 1 M NaOH solution, respectively. The results showed that polymetallic coating was still intact even after continuous immersion in the alkaline solution for 8 days (192 h) and a longer period in the acidic solution, indicating its excellent chemical stability. All the experimental results indicated that the sheathless interface fabricated by the new method in this study was robust and stable, making it promising for both sensitive and robust CE-MS sample analysis.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127045"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Cysteine (Cys) is involved in many physiological processes. It's challenging to detect Cys selectively as it has similar chemical structure with other biothiols such as homocysteine (Hcy) and glutathione (GSH). In this work, a novel fluorescence probe toward mitochondrial cysteine, HPXI-6C, has been developed by employing carbonate as a new recognizing unit and hemicyanine as a chromophore. HPXI-6C exhibits a high selectivity to Cys over hydrogen sulfide, homocysteine and glutathione. The limit of detection toward Cys was determined to be 42 nM. HPXI-6C can localize in mitochondria and produce strong fluorescence peaked at 725 nm in response to Cys in tumor cells. The uptake and generation pathways of Cys in acetaminophen hepatotoxicity cells was revealed by using HPXI-6C. HPXI-6C has been successfully applied in imaging of Cys in drug-induced liver injury in vivo. The research demonstrated that HPXI-6C is powerful in monitoring Cys and is conducive to the early diagnosis of drug-induced liver injury diseases.
{"title":"A selective mitochondria-targeted fluorescent probe for imaging cysteine in drug-induced liver injury.","authors":"Guixin Qin, Lingli Gao, Nan Yin, Mingxiu Wang, Yuting Wang, Jiali Tang, Jianhua Gong, Qingling Xu","doi":"10.1016/j.talanta.2024.127056","DOIUrl":"10.1016/j.talanta.2024.127056","url":null,"abstract":"<p><p>Cysteine (Cys) is involved in many physiological processes. It's challenging to detect Cys selectively as it has similar chemical structure with other biothiols such as homocysteine (Hcy) and glutathione (GSH). In this work, a novel fluorescence probe toward mitochondrial cysteine, HPXI-6C, has been developed by employing carbonate as a new recognizing unit and hemicyanine as a chromophore. HPXI-6C exhibits a high selectivity to Cys over hydrogen sulfide, homocysteine and glutathione. The limit of detection toward Cys was determined to be 42 nM. HPXI-6C can localize in mitochondria and produce strong fluorescence peaked at 725 nm in response to Cys in tumor cells. The uptake and generation pathways of Cys in acetaminophen hepatotoxicity cells was revealed by using HPXI-6C. HPXI-6C has been successfully applied in imaging of Cys in drug-induced liver injury in vivo. The research demonstrated that HPXI-6C is powerful in monitoring Cys and is conducive to the early diagnosis of drug-induced liver injury diseases.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127056"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-10-16DOI: 10.1016/j.talanta.2024.127048
Jun Wang, Jing Ren, Yutong An, Xinyue Xu, Shiqi Yin, Liantao Xin, Hui Zhang, Qingxian Yu, Tianrong Zhan
Herein, we report a fast (10 min) and simple surface treatment of pure carbon cloth (CC) only by an air plasma. The structural characterizations indicate that the air plasma process brings out higher rugosity, more defects, and increased oxygen-related groups on CC surfaces than Ar- or N2-plasma, which can offer abundant capture sites, large electroactive area, and superhydrophilic interface for analytes. As a result, the air-treated CC (CC-PAir) electrode achieves a pronounced improvement of electrocatalytic activity for the [Fe(CN)6]3-/[Fe(CN)6]4- probe evidenced by increased peak currents, decreased peak-to-peak separation, and the lowered resistance of charge transfer. It is also demonstrated that the self-supported CC-PAir electrode possesses excellent sensing performance toward dopamine (DA) and uric acid (UA). The feasibility of the simultaneous electrochemical detection of DA and UA can be verified by their large peak potential gap (∼112 mV) for differential pulse voltammetry. The chronoamperometric sensor yields wide linear ranges of 0.05-100 μM for DA and 0.5-300 μM for UA. The corresponding detection limits are estimated to be 2.6 and 20.4 nM for DA and UA, respectively. The sensor also displays satisfactory selectivity, stability, and reproducibility. Due to good flexibility, the CC-PAir electrode presents great potential for manufacturing wearable and soft electronics for human health monitoring.
在此,我们报告了一种仅用空气等离子体对纯碳布(CC)进行快速(10 分钟)和简单表面处理的方法。结构表征表明,与氩等离子体或二氧化氮等离子体相比,空气等离子体工艺能在 CC 表面产生更高的凹凸度、更多的缺陷和更多的氧相关基团,从而为分析物提供丰富的捕获位点、大面积的电活性区和超亲水界面。因此,经过空气处理的 CC(CC-PAir)电极明显提高了[Fe(CN)6]3-/[Fe(CN)6]4-探针的电催化活性,表现为峰值电流增加、峰-峰分离减小以及电荷转移阻力减小。研究还表明,自支撑 CC-PAir 电极对多巴胺(DA)和尿酸(UA)具有优异的传感性能。在差分脉冲伏安法中,DA 和 UA 的峰值电位差较大(∼112 mV),这验证了同时电化学检测这两种物质的可行性。该计时器传感器的线性范围很宽,DA 为 0.05-100 μM,UA 为 0.5-300 μM。DA 和 UA 的相应检测限估计分别为 2.6 和 20.4 nM。该传感器还具有令人满意的选择性、稳定性和再现性。由于具有良好的灵活性,CC-PAir 电极在制造用于人体健康监测的可穿戴和软电子设备方面具有巨大的潜力。
{"title":"Air plasma fast-induced defect-enriched carbon cloth for simultaneous electrochemical detection of dopamine and uric acid.","authors":"Jun Wang, Jing Ren, Yutong An, Xinyue Xu, Shiqi Yin, Liantao Xin, Hui Zhang, Qingxian Yu, Tianrong Zhan","doi":"10.1016/j.talanta.2024.127048","DOIUrl":"10.1016/j.talanta.2024.127048","url":null,"abstract":"<p><p>Herein, we report a fast (10 min) and simple surface treatment of pure carbon cloth (CC) only by an air plasma. The structural characterizations indicate that the air plasma process brings out higher rugosity, more defects, and increased oxygen-related groups on CC surfaces than Ar- or N<sub>2</sub>-plasma, which can offer abundant capture sites, large electroactive area, and superhydrophilic interface for analytes. As a result, the air-treated CC (CC-P<sub>Air</sub>) electrode achieves a pronounced improvement of electrocatalytic activity for the [Fe(CN)<sub>6</sub>]<sup>3-</sup>/[Fe(CN)<sub>6</sub>]<sup>4-</sup> probe evidenced by increased peak currents, decreased peak-to-peak separation, and the lowered resistance of charge transfer. It is also demonstrated that the self-supported CC-P<sub>Air</sub> electrode possesses excellent sensing performance toward dopamine (DA) and uric acid (UA). The feasibility of the simultaneous electrochemical detection of DA and UA can be verified by their large peak potential gap (∼112 mV) for differential pulse voltammetry. The chronoamperometric sensor yields wide linear ranges of 0.05-100 μM for DA and 0.5-300 μM for UA. The corresponding detection limits are estimated to be 2.6 and 20.4 nM for DA and UA, respectively. The sensor also displays satisfactory selectivity, stability, and reproducibility. Due to good flexibility, the CC-P<sub>Air</sub> electrode presents great potential for manufacturing wearable and soft electronics for human health monitoring.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"282 ","pages":"127048"},"PeriodicalIF":8.3,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}