For patients with chronic spinal cord injury,the co nventional treatment is rehabilitation and treatment of spinal cord injury complications such as urinary tract infection,pressure sores,osteoporosis,and deep vein th...For patients with chronic spinal cord injury,the co nventional treatment is rehabilitation and treatment of spinal cord injury complications such as urinary tract infection,pressure sores,osteoporosis,and deep vein thrombosis.Surgery is rarely perfo rmed on spinal co rd injury in the chronic phase,and few treatments have been proven effective in chronic spinal cord injury patients.Development of effective therapies fo r chronic spinal co rd injury patients is needed.We conducted a randomized controlled clinical trial in patients with chronic complete thoracic spinal co rd injury to compare intensive rehabilitation(weight-bearing walking training)alone with surgical intervention plus intensive rehabilitation.This clinical trial was registered at ClinicalTrials.gov(NCT02663310).The goal of surgical intervention was spinal cord detethering,restoration of cerebrospinal fluid flow,and elimination of residual spinal cord compression.We found that surgical intervention plus weight-bearing walking training was associated with a higher incidence of American Spinal Injury Association Impairment Scale improvement,reduced spasticity,and more rapid bowel and bladder functional recovery than weight-bearing walking training alone.Overall,the surgical procedures and intensive rehabilitation were safe.American Spinal Injury Association Impairment Scale improvement was more common in T7-T11 injuries than in T2-T6 injuries.Surgery combined with rehabilitation appears to have a role in treatment of chronic spinal cord injury patients.展开更多
The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fab...The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.展开更多
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding...Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.展开更多
Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This articl...Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution,and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.The images or other third-party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.展开更多
Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of cata...Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.展开更多
基金supported by Hong Kong Spinal Cord Injury Fund (HKSCIF),China (to HZ)。
文摘For patients with chronic spinal cord injury,the co nventional treatment is rehabilitation and treatment of spinal cord injury complications such as urinary tract infection,pressure sores,osteoporosis,and deep vein thrombosis.Surgery is rarely perfo rmed on spinal co rd injury in the chronic phase,and few treatments have been proven effective in chronic spinal cord injury patients.Development of effective therapies fo r chronic spinal co rd injury patients is needed.We conducted a randomized controlled clinical trial in patients with chronic complete thoracic spinal co rd injury to compare intensive rehabilitation(weight-bearing walking training)alone with surgical intervention plus intensive rehabilitation.This clinical trial was registered at ClinicalTrials.gov(NCT02663310).The goal of surgical intervention was spinal cord detethering,restoration of cerebrospinal fluid flow,and elimination of residual spinal cord compression.We found that surgical intervention plus weight-bearing walking training was associated with a higher incidence of American Spinal Injury Association Impairment Scale improvement,reduced spasticity,and more rapid bowel and bladder functional recovery than weight-bearing walking training alone.Overall,the surgical procedures and intensive rehabilitation were safe.American Spinal Injury Association Impairment Scale improvement was more common in T7-T11 injuries than in T2-T6 injuries.Surgery combined with rehabilitation appears to have a role in treatment of chronic spinal cord injury patients.
基金The authors are grateful for the financial support from the National Natural Science Foundation of China(Grant Nos.52273067,52122303,52233006)the Fundamental Research Funds for the Central Universities(Grant No.2232023A-03)the Shuguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(23SG29).
文摘The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
基金financially suppor ted by Key Research and Development Project of Anhui Province(No.2023h11020002)Natural Science Research Project for Universities in Anhui Province(No.KJ2021ZD0006)+3 种基金Natural Science Foundation of Anhui Province(No.2208085MB21)Fundamental Research Funds for the Central Universities of China(No.PA2022GDSK0056)Anhui Laboratory of Molecule-Based Materials(No.fzj22009)National Natural Science Foundation of China(Nos.21725102,22205108)。
文摘Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.
文摘Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution,and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.The images or other third-party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.
基金financially supported by the National Natural Science Foundation of China (22172044 and 22208048)Heilongjiang Provincial Natural Science Foundation of China (YQ2022B005 and YQ2022B001)+4 种基金the Young Elite Scientists Sponsorship Program by CAST (No.YESS20210262)the China Postdoctoral Science Foundation-Funded Project (No.2021M690571)the Heilongjiang Postdoctoral Fund (No.LBH-Z21096)the Provincial Natural Science Foundation Joint Guidance Project (No.LH2020F001)the Fundamental Research Funds for the Central Universities (No.2572023CT10)。
文摘Single-atom catalysts(SACs)are gaining popularity in catalytic reactions due to their nearly 100%atomic utilization and defined active sites,which provide great convenience for studying the catalytic mechanism of catalysts.However,SACs still present challenges such as complex formation processes,low loading and easy agglomeration of catalysts.Herein,we systematically discuss the synthesis methods for SACs,including coprecipitation,impregnation,atomic layer deposition,pyrolysis and Anti-Ostwald ripening etc.Various techniques for characterizing single-atom catalysts(SACs)are described in detail.The utilization of individual atoms in various photocatalytic reactions and their mechanisms of action in different reactions are explained.The purpose of this review is to introduce single-atom synthesis methods,characterization techniques,specific catalytic action and their applications in the direction of photocatalysis,and to provide a reference for the industrialization of photocatalytic single-atoms,which is currently impossible,in the hope of promoting further development of photocatalytic single-atoms.
