Veronica Di Battista, Pernille Høgh Danielsen, Agnieszka Gajewicz-Skretna, Andrzej Kedziorski, Svenja B. Seiffert, Lan Ma-Hock, Trine Berthing, Alicja Mortensen, Andreas Sundermann, Lars Michael Skjolding, Ulla Vogel, Anders Baun, Wendel Wohlleben
Oxide-perovskites designed for automotive catalysts contain multiple metal elements whose presence is crucial to achieving the targeted performance. They are highly stable in exhaust operating conditions; however, little is known about their stability under physiological conditions. As some of the metallic components are hazardous to humans and the environment, perovskite benefits in cleaner air must be balanced with risks in a Safe and Sustainable Design (SSbD) approach. New approach methodologies (NAMs), including in chemico and in silico methods, were used for testing hazards and benefits, including catalytic activity and tolerance for temporary excess of oxygen under dynamic driving conditions. The composition and surface properties of six different lanthanum-based oxide-perovskites compromised their stability under lung physiological conditions, influencing the oxidative damage of the particles and the bioacessibility of leaching metals. We found consistent biotransformation of the oxide-perovskite materials at pH 4.5. The leached lanthanum ions, but not other metals, respeciated into lanthanum phosphate nanoparticles, which increased the overall oxidative damage in additive synergy. The NAM results in the presented SSbD approach were challenged by in vivo studies in rats and mice, which confirmed multicomponent clearance from lungs into urine and supported the comparative ranking of effects against well-characterized spinel materials. Among the perovskites, the version with reduced nickel content and doped with palladium offered the best SSbD balance, despite not improving the conventional benchmark catalytic performance and related sustainability benefits. Redesign by industry may be necessary to better fulfill all SSbD dimensions.
{"title":"Oxide-Perovskites for Automotive Catalysts Biotransform and Induce Multicomponent Clearance and Hazard","authors":"Veronica Di Battista, Pernille Høgh Danielsen, Agnieszka Gajewicz-Skretna, Andrzej Kedziorski, Svenja B. Seiffert, Lan Ma-Hock, Trine Berthing, Alicja Mortensen, Andreas Sundermann, Lars Michael Skjolding, Ulla Vogel, Anders Baun, Wendel Wohlleben","doi":"10.1021/acsnano.4c10135","DOIUrl":"https://doi.org/10.1021/acsnano.4c10135","url":null,"abstract":"Oxide-perovskites designed for automotive catalysts contain multiple metal elements whose presence is crucial to achieving the targeted performance. They are highly stable in exhaust operating conditions; however, little is known about their stability under physiological conditions. As some of the metallic components are hazardous to humans and the environment, perovskite benefits in cleaner air must be balanced with risks in a Safe and Sustainable Design (SSbD) approach. New approach methodologies (NAMs), including in chemico and in silico methods, were used for testing hazards and benefits, including catalytic activity and tolerance for temporary excess of oxygen under dynamic driving conditions. The composition and surface properties of six different lanthanum-based oxide-perovskites compromised their stability under lung physiological conditions, influencing the oxidative damage of the particles and the bioacessibility of leaching metals. We found consistent biotransformation of the oxide-perovskite materials at pH 4.5. The leached lanthanum ions, but not other metals, respeciated into lanthanum phosphate nanoparticles, which increased the overall oxidative damage in additive synergy. The NAM results in the presented SSbD approach were challenged by in vivo studies in rats and mice, which confirmed multicomponent clearance from lungs into urine and supported the comparative ranking of effects against well-characterized spinel materials. Among the perovskites, the version with reduced nickel content and doped with palladium offered the best SSbD balance, despite not improving the conventional benchmark catalytic performance and related sustainability benefits. Redesign by industry may be necessary to better fulfill all SSbD dimensions.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"16 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1126/scitranslmed.adr1032
Rebecca E. Hamlin, Shaun M. Pienkos, Leslie Chan, Mikayla A. Stabile, Kassandra Pinedo, Mallika Rao, Philip Grant, Hector Bonilla, Marisa Holubar, Upinder Singh, Karen B. Jacobson, Prasanna Jagannathan, Yvonne Maldonado, Susan P. Holmes, Aruna Subramanian, Catherine A. Blish
Sex differences have been observed in acute coronavirus disease 2019 (COVID-19) and Long Covid (LC) outcomes, with greater disease severity and mortality during acute infection in males and greater proportions of females developing LC. We hypothesized that sex-specific immune dysregulation contributes to LC pathogenesis. To investigate the immunologic underpinnings of LC development and symptom persistence, we performed multiomic analyses on blood samples obtained during acute severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) infection and 3 and 12 months after infection in a cohort of 45 participants who either developed LC or recovered. Several sex-specific immune pathways were associated with LC. Males who would later develop LC exhibited increases in transforming growth factor–β (TGF-β) signaling during acute infection, whereas females who would go on to develop LC had reduced TGFB1 expression. Females who developed LC demonstrated increased expression of XIST , an RNA gene implicated in autoimmunity, during acute infection compared with females who recovered. Many immune features of LC were also conserved across sexes, such as alterations in monocyte phenotype and activation state. Nuclear factor κB (NF-κB) transcription factors were up-regulated in many cell types at acute and convalescent time points. Those with ongoing LC demonstrated reduced ETS1 expression across lymphocyte subsets and elevated intracellular IL-4 in T cell subsets, suggesting that ETS1 alterations may drive aberrantly elevated T helper cell 2–like responses in LC. Altogether, this study describes multiple innate and adaptive immune correlates of LC, some of which differ by sex, and offers insights toward the pursuit of tailored therapeutics.
{"title":"Sex differences and immune correlates of Long Covid development, symptom persistence, and resolution","authors":"Rebecca E. Hamlin, Shaun M. Pienkos, Leslie Chan, Mikayla A. Stabile, Kassandra Pinedo, Mallika Rao, Philip Grant, Hector Bonilla, Marisa Holubar, Upinder Singh, Karen B. Jacobson, Prasanna Jagannathan, Yvonne Maldonado, Susan P. Holmes, Aruna Subramanian, Catherine A. Blish","doi":"10.1126/scitranslmed.adr1032","DOIUrl":"https://doi.org/10.1126/scitranslmed.adr1032","url":null,"abstract":"Sex differences have been observed in acute coronavirus disease 2019 (COVID-19) and Long Covid (LC) outcomes, with greater disease severity and mortality during acute infection in males and greater proportions of females developing LC. We hypothesized that sex-specific immune dysregulation contributes to LC pathogenesis. To investigate the immunologic underpinnings of LC development and symptom persistence, we performed multiomic analyses on blood samples obtained during acute severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) infection and 3 and 12 months after infection in a cohort of 45 participants who either developed LC or recovered. Several sex-specific immune pathways were associated with LC. Males who would later develop LC exhibited increases in transforming growth factor–β (TGF-β) signaling during acute infection, whereas females who would go on to develop LC had reduced <jats:italic>TGFB1</jats:italic> expression. Females who developed LC demonstrated increased expression of <jats:italic>XIST</jats:italic> , an RNA gene implicated in autoimmunity, during acute infection compared with females who recovered. Many immune features of LC were also conserved across sexes, such as alterations in monocyte phenotype and activation state. Nuclear factor κB (NF-κB) transcription factors were up-regulated in many cell types at acute and convalescent time points. Those with ongoing LC demonstrated reduced <jats:italic>ETS1</jats:italic> expression across lymphocyte subsets and elevated intracellular IL-4 in T cell subsets, suggesting that <jats:italic>ETS1</jats:italic> alterations may drive aberrantly elevated T helper cell 2–like responses in LC. Altogether, this study describes multiple innate and adaptive immune correlates of LC, some of which differ by sex, and offers insights toward the pursuit of tailored therapeutics.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1126/scitranslmed.ado2102
Julio Silva, Akiko Iwasaki
Postacute infection syndromes like Long Covid disproportionately affect females, differing in prevalence, symptoms, and potential causes from males. This Viewpoint highlights these sex differences, gaps in current understanding, and the critical need for sex-based research.
像 Long Covid 这样的急性感染后综合征对女性的影响尤为严重,在发病率、症状和潜在病因方面都与男性不同。本视点强调了这些性别差异、目前认识上的差距以及基于性别进行研究的迫切需要。
{"title":"Sex differences in postacute infection syndromes","authors":"Julio Silva, Akiko Iwasaki","doi":"10.1126/scitranslmed.ado2102","DOIUrl":"https://doi.org/10.1126/scitranslmed.ado2102","url":null,"abstract":"Postacute infection syndromes like Long Covid disproportionately affect females, differing in prevalence, symptoms, and potential causes from males. This Viewpoint highlights these sex differences, gaps in current understanding, and the critical need for sex-based research.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"63 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Extracellular vesicles (EVs) hosting enzymatic activities that function as independent metabolic units are attractive natural biocatalytic platforms. However, directly using these metabolically active nanoreactors for effective biocatalytic applications remains challenging, mainly due to their constrained catalytic capabilities. Here, we construct an EV-templated nanobiohybrid system by engineering an EV surface with a photoresponsive zeolitic imidazolate framework (ZIF). The deposition of ZIF nanostructures on EVs not only contributes to improved biocatalytic stability but also enables interfacial coupling between photoexcited electrons from the ZIF and the enzymatic reaction of metabolically active EVs. Nearly 300% of biomass conversion efficiency increment could be achieved by EVs derived from macrophages. This enhanced biocatalysis, high catalytic stability, and low cytotoxicity endowed the EV@ZIF nanosystem with robust biosynthesis and antimicrobial activity. When evaluated in a mouse periodontitis model, we show that the autologous biocatalytic EV@ZIF demonstrated efficient therapeutic capability by killing bacteria and inhibiting inflammation. This nanoengineering strategy will benefit the future optimization of metabolically active EV nanoreactors as biocatalysts for a broad range of therapeutics.
细胞外囊泡(EVs)具有作为独立代谢单元的酶活性,是极具吸引力的天然生物催化平台。然而,直接利用这些具有代谢活性的纳米反应器进行有效的生物催化应用仍然具有挑战性,这主要是由于它们的催化能力受到限制。在这里,我们通过用具有光致伸缩性的唑基咪唑啉框架(ZIF)对电动汽车表面进行工程化处理,构建了一个电动汽车模板纳米生物杂交系统。在 EV 上沉积 ZIF 纳米结构不仅有助于提高生物催化稳定性,还能使 ZIF 的光激发电子与代谢活跃的 EV 的酶反应发生界面耦合。来自巨噬细胞的 EVs 可使生物质转化效率提高近 300%。这种增强的生物催化作用、高催化稳定性和低细胞毒性赋予了 EV@ZIF 纳米系统强大的生物合成和抗菌活性。在小鼠牙周炎模型中进行评估时,我们发现自体生物催化 EV@ZIF 通过杀死细菌和抑制炎症表现出高效的治疗能力。这种纳米工程策略将有助于优化具有代谢活性的 EV 纳米反应器,使其成为广泛治疗的生物催化剂。
{"title":"Nanobiohybrid Extracellular Vesicle Nanoreactor with Improving Metabolical Activity for Biocatalytic Therapy","authors":"Shuangshuang Wan, Wurui Liu, Qian Wu, Kepeng Wang, Yaocheng Li, Peihong Huang, Yu Wu, Yunfei Mu, Yulin Fan, Jun Tao, Jia Yao, Fei Peng, Yu Zou, Lianhui Wang, Zhiyao Yuan, Xianguang Ding","doi":"10.1021/acsnano.4c12458","DOIUrl":"https://doi.org/10.1021/acsnano.4c12458","url":null,"abstract":"Extracellular vesicles (EVs) hosting enzymatic activities that function as independent metabolic units are attractive natural biocatalytic platforms. However, directly using these metabolically active nanoreactors for effective biocatalytic applications remains challenging, mainly due to their constrained catalytic capabilities. Here, we construct an EV-templated nanobiohybrid system by engineering an EV surface with a photoresponsive zeolitic imidazolate framework (ZIF). The deposition of ZIF nanostructures on EVs not only contributes to improved biocatalytic stability but also enables interfacial coupling between photoexcited electrons from the ZIF and the enzymatic reaction of metabolically active EVs. Nearly 300% of biomass conversion efficiency increment could be achieved by EVs derived from macrophages. This enhanced biocatalysis, high catalytic stability, and low cytotoxicity endowed the EV@ZIF nanosystem with robust biosynthesis and antimicrobial activity. When evaluated in a mouse periodontitis model, we show that the autologous biocatalytic EV@ZIF demonstrated efficient therapeutic capability by killing bacteria and inhibiting inflammation. This nanoengineering strategy will benefit the future optimization of metabolically active EV nanoreactors as biocatalysts for a broad range of therapeutics.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"98 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609857","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1001/jamasurg.2024.5091
Brian T. Fry, Leah J. Schoel, Ryan A. Howard, Jyothi R. Thumma, Abigail L. Kappelman, Alexander K. Hallway, Anne P. Ehlers, Sean M. O’Neill, Michael A. Rubyan, Jenny M. Shao, Dana A. Telem
ImportanceComponent separation is a reconstructive technique used to facilitate midline closure of large or complex ventral hernias. Despite a contemporary surge in popularity, the incidence and long-term outcomes after component separation remain unknown.ObjectiveTo evaluate the incidence and long-term outcomes of component separation for abdominal wall hernia repair.Design, Setting, and ParticipantsThis cohort study examined 100% Medicare administrative claims data from January 1, 2007, to December 31, 2021. Participants were adults (aged ≥18 years) who underwent elective inpatient ventral hernia repair. Data were analyzed from January through June 2024.ExposureUse of component separation technique during ventral hernia repair.Main Outcomes and MeasuresThe primary outcomes were the incidence of component separation over time and operative recurrence rates up to 10 years after surgery for hernia repairs with and without component separation. The secondary outcome was rate of operative recurrence after component separation stratified by surgeon volume.ResultsAmong 218 518 patients who underwent ventral hernia repair, the mean (SD) age of the cohort was 69.1 (10.9) years; 127 857 patients (58.5%) were female and 90 661 (41.5%) male. A total of 23 768 individuals had component separation for their abdominal wall hernia repair. The median (IQR) follow-up time after the index hernia surgery was 7.2 (2.7-10) years. Compared with patients who did not have a component separation, patients undergoing repair with component separation were slightly younger; more likely to be male; and more likely to have comorbidities, including obesity, and had surgeries that were more likely to be performed open and use mesh. Proportional use of component separation increased from 1.6% of all inpatient hernia repairs in 2007 (279 patients) to 21.4% in 2021 (1569 patients). The 10-year adjusted operative recurrence rate after component separation was lower (11.2%; 95% CI, 11.0%-11.3%) when compared with hernia repairs performed without component separation (12.9%; 95% CI, 12.8%-13.0%; P = .003). Operative recurrence was lower for the top 5% of surgeons by component separation volume (11.9%; 95% CI, 11.8%-12.1%) as opposed to the bottom 95% of surgeons by volume (13.6%; 95% CI, 13.4%-13.7%; P = .004).Conclusions and RelevanceThis study found that component separation was associated with a protective effect on long-term operative recurrence after ventral hernia repair among Medicare beneficiaries, which is somewhat unexpected given the intent of its use for higher complexity hernias. Surgeon volume, while significant, had only a minor influence on operative recurrence rates.
{"title":"Long-Term Outcomes of Component Separation for Abdominal Wall Hernia Repair","authors":"Brian T. Fry, Leah J. Schoel, Ryan A. Howard, Jyothi R. Thumma, Abigail L. Kappelman, Alexander K. Hallway, Anne P. Ehlers, Sean M. O’Neill, Michael A. Rubyan, Jenny M. Shao, Dana A. Telem","doi":"10.1001/jamasurg.2024.5091","DOIUrl":"https://doi.org/10.1001/jamasurg.2024.5091","url":null,"abstract":"ImportanceComponent separation is a reconstructive technique used to facilitate midline closure of large or complex ventral hernias. Despite a contemporary surge in popularity, the incidence and long-term outcomes after component separation remain unknown.ObjectiveTo evaluate the incidence and long-term outcomes of component separation for abdominal wall hernia repair.Design, Setting, and ParticipantsThis cohort study examined 100% Medicare administrative claims data from January 1, 2007, to December 31, 2021. Participants were adults (aged ≥18 years) who underwent elective inpatient ventral hernia repair. Data were analyzed from January through June 2024.ExposureUse of component separation technique during ventral hernia repair.Main Outcomes and MeasuresThe primary outcomes were the incidence of component separation over time and operative recurrence rates up to 10 years after surgery for hernia repairs with and without component separation. The secondary outcome was rate of operative recurrence after component separation stratified by surgeon volume.ResultsAmong 218 518 patients who underwent ventral hernia repair, the mean (SD) age of the cohort was 69.1 (10.9) years; 127 857 patients (58.5%) were female and 90 661 (41.5%) male. A total of 23 768 individuals had component separation for their abdominal wall hernia repair. The median (IQR) follow-up time after the index hernia surgery was 7.2 (2.7-10) years. Compared with patients who did not have a component separation, patients undergoing repair with component separation were slightly younger; more likely to be male; and more likely to have comorbidities, including obesity, and had surgeries that were more likely to be performed open and use mesh. Proportional use of component separation increased from 1.6% of all inpatient hernia repairs in 2007 (279 patients) to 21.4% in 2021 (1569 patients). The 10-year adjusted operative recurrence rate after component separation was lower (11.2%; 95% CI, 11.0%-11.3%) when compared with hernia repairs performed without component separation (12.9%; 95% CI, 12.8%-13.0%; <jats:italic>P</jats:italic> = .003). Operative recurrence was lower for the top 5% of surgeons by component separation volume (11.9%; 95% CI, 11.8%-12.1%) as opposed to the bottom 95% of surgeons by volume (13.6%; 95% CI, 13.4%-13.7%; <jats:italic>P</jats:italic> = .004).Conclusions and RelevanceThis study found that component separation was associated with a protective effect on long-term operative recurrence after ventral hernia repair among Medicare beneficiaries, which is somewhat unexpected given the intent of its use for higher complexity hernias. Surgeon volume, while significant, had only a minor influence on operative recurrence rates.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"108 1","pages":""},"PeriodicalIF":16.9,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Zhao, Xiaohui Zhu, Qinghua Zhang, Lin Gu, Zhengyi Shi, Ce Qiu, Tingting Chen, Mingzhu Ni, Yuhang Zhuang, Serguei V. Savilov, Sergey M. Aldoshin, Hui Xia
Layered Na-birnessites are promising cathode materials for aqueous sodium-ion batteries due to their high theoretical capacity, low cost, and environmental benignity. However, the general O′3 Na-birnessites possess low Na content and dominant inactive {001} exposed facets, which compromise their Na storage capability and cycling stability. Herein, we develop a high-Na-content P′3-Na0.71MnO2·0.15H2O with highly enriched {010} active facets by a hydrothermal conversion method. In comparison with the O′3 Na-birnessite, the P′3 Na-birnessite with a high ratio of {010}/{001} exposed facets provides greatly increased open channels for Na+ diffusion, while the P′3 stacking affords a lower Na+ diffusion barrier, resulting in improved electrode kinetics with a large specific capacity of 176 mAh g–1 at 0.2 A g–1. More importantly, the P′3 Na-birnessite manifests solo Na+ intercalation/deintercalation with extraordinary cycling stability in an aqueous electrolyte, achieving 90.5% capacity retention after 60,000 cycles. When coupled with the NaTi2(PO4)3 anode, the P′3 Na-birnessite-based full cell delivers both high energy density and long cycle life, demonstrating the potential application in aqueous sodium-ion batteries. This study demonstrates an efficient method to prepare high-Na-content P′3 birnessite with tunable exposed facets and provides important insights into developing highly stable layered cathodes for sustainable aqueous sodium-ion batteries.
{"title":"High-Na-Content Birnessite via P′3-Stacking with Tunable Active Facets for Advanced Aqueous Sodium-Ion Batteries","authors":"Yang Zhao, Xiaohui Zhu, Qinghua Zhang, Lin Gu, Zhengyi Shi, Ce Qiu, Tingting Chen, Mingzhu Ni, Yuhang Zhuang, Serguei V. Savilov, Sergey M. Aldoshin, Hui Xia","doi":"10.1021/acsnano.4c09448","DOIUrl":"https://doi.org/10.1021/acsnano.4c09448","url":null,"abstract":"Layered Na-birnessites are promising cathode materials for aqueous sodium-ion batteries due to their high theoretical capacity, low cost, and environmental benignity. However, the general O′3 Na-birnessites possess low Na content and dominant inactive {001} exposed facets, which compromise their Na storage capability and cycling stability. Herein, we develop a high-Na-content P′3-Na<sub>0.71</sub>MnO<sub>2</sub>·0.15H<sub>2</sub>O with highly enriched {010} active facets by a hydrothermal conversion method. In comparison with the O′3 Na-birnessite, the P′3 Na-birnessite with a high ratio of {010}/{001} exposed facets provides greatly increased open channels for Na<sup>+</sup> diffusion, while the P′3 stacking affords a lower Na<sup>+</sup> diffusion barrier, resulting in improved electrode kinetics with a large specific capacity of 176 mAh g<sup>–1</sup> at 0.2 A g<sup>–1</sup>. More importantly, the P′3 Na-birnessite manifests solo Na<sup>+</sup> intercalation/deintercalation with extraordinary cycling stability in an aqueous electrolyte, achieving 90.5% capacity retention after 60,000 cycles. When coupled with the NaTi<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> anode, the P′3 Na-birnessite-based full cell delivers both high energy density and long cycle life, demonstrating the potential application in aqueous sodium-ion batteries. This study demonstrates an efficient method to prepare high-Na-content P′3 birnessite with tunable exposed facets and provides important insights into developing highly stable layered cathodes for sustainable aqueous sodium-ion batteries.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1001/jamasurg.2024.4522
Danielle Brabender, Kazuhide Matsushima, Morgan Schellenberg, Kenji Inaba, Charles Wade, John B. Holcomb, Matthew Martin
This comparative effectiveness research uses data from the Pragmatic, Randomized Optimal Platelet and Plasma Ratios (PROPPR) randomized clinical trial to compare benefits with balanced resuscitation for thoracic vs abdominopelvic traumatic hemorrhage.
{"title":"Benefits of Different Balanced Resuscitation Ratios for Thoracic vs Abdominopelvic Traumatic Hemorrhage","authors":"Danielle Brabender, Kazuhide Matsushima, Morgan Schellenberg, Kenji Inaba, Charles Wade, John B. Holcomb, Matthew Martin","doi":"10.1001/jamasurg.2024.4522","DOIUrl":"https://doi.org/10.1001/jamasurg.2024.4522","url":null,"abstract":"This comparative effectiveness research uses data from the Pragmatic, Randomized Optimal Platelet and Plasma Ratios (PROPPR) randomized clinical trial to compare benefits with balanced resuscitation for thoracic vs abdominopelvic traumatic hemorrhage.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"34 1","pages":""},"PeriodicalIF":16.9,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1001/jamasurg.2024.4811
Thomas Li, Sunny Nalavenkata, Jonathan Fainberg
ImportanceActive surveillance (AS) has become an increasingly important option for managing low-risk and select intermediate-risk prostate cancer. Although imaging, particularly multiparametric magnetic resonance imaging (mpMRI), has emerged in the prebiopsy pathway for the diagnosis of prostate cancer, the role of mpMRI in patient selection for AS and the necessity of prostate biopsies during AS remain poorly defined. Despite well-founded biopsy schedules, there has been substantial investigation into whether imaging may supplant the need for prostate biopsies during AS. This review aimed to summarize the contemporary role of imaging in the diagnosis and surveillance of prostate cancer.ObservationsMultiparametric MRI is the most established form of imaging in prostate cancer, with routine prebiopsy use being shown to help urologists distinguish between clinically significant and clinically insignificant disease. The visibility of these lesions on mpMRI closely correlates with their behavior, with visible disease portending a worse prognosis. Combined with other clinical data, risk calculators may better delineate patients with higher-risk disease and exclude them from undergoing AS. While current evidence suggests that mpMRI cannot replace the need for prostate biopsy during AS due to the possibility of missing higher-risk disease, the addition of prostate biomarkers may help to reduce the frequency of these biopsies. The role of prostate-specific antigen positron emission tomography/computed tomography is still emerging but has shown promising early results as an adjunct to mpMRI in initial diagnosis.Conclusions and RelevanceImaging in prostate cancer helps to better select patients appropriate for AS, and future studies may strengthen the predictive capabilities of risk calculators. Multiparametric MRI has been shown to be imperative to rationalizing biopsies for patients enrolled in AS. However, heterogeneity in the evidence of mpMRI during AS has suggested that further prospective studies and randomized clinical trials, particularly in homogenizing reporting standards, may reveal a more defined role in monitoring disease progression.
{"title":"Imaging in Diagnosis and Active Surveillance for Prostate Cancer","authors":"Thomas Li, Sunny Nalavenkata, Jonathan Fainberg","doi":"10.1001/jamasurg.2024.4811","DOIUrl":"https://doi.org/10.1001/jamasurg.2024.4811","url":null,"abstract":"ImportanceActive surveillance (AS) has become an increasingly important option for managing low-risk and select intermediate-risk prostate cancer. Although imaging, particularly multiparametric magnetic resonance imaging (mpMRI), has emerged in the prebiopsy pathway for the diagnosis of prostate cancer, the role of mpMRI in patient selection for AS and the necessity of prostate biopsies during AS remain poorly defined. Despite well-founded biopsy schedules, there has been substantial investigation into whether imaging may supplant the need for prostate biopsies during AS. This review aimed to summarize the contemporary role of imaging in the diagnosis and surveillance of prostate cancer.ObservationsMultiparametric MRI is the most established form of imaging in prostate cancer, with routine prebiopsy use being shown to help urologists distinguish between clinically significant and clinically insignificant disease. The visibility of these lesions on mpMRI closely correlates with their behavior, with visible disease portending a worse prognosis. Combined with other clinical data, risk calculators may better delineate patients with higher-risk disease and exclude them from undergoing AS. While current evidence suggests that mpMRI cannot replace the need for prostate biopsy during AS due to the possibility of missing higher-risk disease, the addition of prostate biomarkers may help to reduce the frequency of these biopsies. The role of prostate-specific antigen positron emission tomography/computed tomography is still emerging but has shown promising early results as an adjunct to mpMRI in initial diagnosis.Conclusions and RelevanceImaging in prostate cancer helps to better select patients appropriate for AS, and future studies may strengthen the predictive capabilities of risk calculators. Multiparametric MRI has been shown to be imperative to rationalizing biopsies for patients enrolled in AS. However, heterogeneity in the evidence of mpMRI during AS has suggested that further prospective studies and randomized clinical trials, particularly in homogenizing reporting standards, may reveal a more defined role in monitoring disease progression.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"20 1","pages":""},"PeriodicalIF":16.9,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601964","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The characteristics of the directed transport of liquids based on Janus membranes play a crucial role in practical applications in energy, materials, physics, chemistry, medicine, biology, and other fields. Although extensive progress has been made, it is still difficult to realize the accurate controllability of liquid directional transmembrane transport. The current gating strategies for the directed transport of liquids based on Janus membranes still have some limitations: (a) using magnetic fluid may cause contamination due to the addition of new substances and (b) utilizing hydrophobicity/hydrophilicity conversion of titanium dioxide requires a long switching time (over 30 min). Herein, a strategy is proposed to precisely control liquid directional transport by altering the wettability of droplets on Janus films prepared by a femtosecond laser through photothermal effects. Infrared laser irradiation on Janus film coated with CNTs can effectively convert light energy into thermal energy, rapidly increase the surface temperature of Janus film, and change the wettability of the liquid on the film. Liquid transmembrane directional transport can be achieved within a few seconds without contaminating the transported liquid. The proposed gating strategy can enable the application of Janus membranes in various scenarios such as microchemical reactions, biological cell culture, and interface self-propulsion.
{"title":"Light-Triggered Droplet Gating Strategy Based on Janus Membrane Fabricated by Femtosecond Laser","authors":"Kangru Cheng, Wenlong Xu, Hao Wu, Bowen Chen, Haoxiang Yang, Zehang Cui, Hao Yu, Zilong Cheng, Yanlei Hu, Jiawen Li, Hongyuan Jiang, Jiaru Chu, Dong Wu","doi":"10.1021/acsnano.4c08108","DOIUrl":"https://doi.org/10.1021/acsnano.4c08108","url":null,"abstract":"The characteristics of the directed transport of liquids based on Janus membranes play a crucial role in practical applications in energy, materials, physics, chemistry, medicine, biology, and other fields. Although extensive progress has been made, it is still difficult to realize the accurate controllability of liquid directional transmembrane transport. The current gating strategies for the directed transport of liquids based on Janus membranes still have some limitations: (a) using magnetic fluid may cause contamination due to the addition of new substances and (b) utilizing hydrophobicity/hydrophilicity conversion of titanium dioxide requires a long switching time (over 30 min). Herein, a strategy is proposed to precisely control liquid directional transport by altering the wettability of droplets on Janus films prepared by a femtosecond laser through photothermal effects. Infrared laser irradiation on Janus film coated with CNTs can effectively convert light energy into thermal energy, rapidly increase the surface temperature of Janus film, and change the wettability of the liquid on the film. Liquid transmembrane directional transport can be achieved within a few seconds without contaminating the transported liquid. The proposed gating strategy can enable the application of Janus membranes in various scenarios such as microchemical reactions, biological cell culture, and interface self-propulsion.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"6 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601572","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
1T-TiSe2, a promising candidate of the sought-after excitonic insulator, possesses an enigmatic charge density wave (CDW) order of which the microscopic origin is formidable to settle owing to the chicken-and-egg entanglement between the electron and lattice degrees of freedom. Its CDW experiences an intriguing but elusive quantum melting and eventually enters the superconducting phase under metal intercalation, suggesting the possible role of melted-order fluctuation in gluing the electron paring. Employing the spectroscopic imaging scanning tunneling microscope (STM), we access the pure electronic behavior by visualizing the CDW melting process of monolayer 1T-TiSe2 in both the space and energy-band dimensions. In real space, the native lattice imperfections disturb the local order parameter and stimulate the melting of CDW. In energy-band space, different states exhibit varying stiffness against the melting stimuli, yielding distinctive melted textures. The evolution of CDW topological defects and the structure factor in the quantum melting process provide a straightforward avenue to evaluate the CDW coherency, which shows that the CDW stiffness scales with the strength of the p-d Coulomb correlation. Our study reveals the quantum melting of CDW with an altering band-orbital-correlation character and puts compelling emphasis on the indispensable role of excitonic interaction in stabilizing the charge order of monolayer TiSe2.
{"title":"P-d Correlation-Determined Charge Order Stiffness and Corresponding Quantum Melting in Monolayer 1T-TiSe2","authors":"Cheng-Yen Liu, Meng Zhao, Zhongjie Wang, Chun-Lei Gao","doi":"10.1021/acsnano.4c11704","DOIUrl":"https://doi.org/10.1021/acsnano.4c11704","url":null,"abstract":"1T-TiSe<sub>2</sub>, a promising candidate of the sought-after excitonic insulator, possesses an enigmatic charge density wave (CDW) order of which the microscopic origin is formidable to settle owing to the chicken-and-egg entanglement between the electron and lattice degrees of freedom. Its CDW experiences an intriguing but elusive quantum melting and eventually enters the superconducting phase under metal intercalation, suggesting the possible role of melted-order fluctuation in gluing the electron paring. Employing the spectroscopic imaging scanning tunneling microscope (STM), we access the pure electronic behavior by visualizing the CDW melting process of monolayer 1T-TiSe<sub>2</sub> in both the space and energy-band dimensions. In real space, the native lattice imperfections disturb the local order parameter and stimulate the melting of CDW. In energy-band space, different states exhibit varying stiffness against the melting stimuli, yielding distinctive melted textures. The evolution of CDW topological defects and the structure factor in the quantum melting process provide a straightforward avenue to evaluate the CDW coherency, which shows that the CDW stiffness scales with the strength of the p-d Coulomb correlation. Our study reveals the quantum melting of CDW with an altering band-orbital-correlation character and puts compelling emphasis on the indispensable role of excitonic interaction in stabilizing the charge order of monolayer TiSe<sub>2</sub>.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"158 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}