Selective oxidation of 5-hydroxymethylfurfual(HMF) to 2,5-furandicarboxylic acid(FDCA) as a bioplastics monomer is efficiently promoted by a simple system without noble-metal and base additives. In this work, graphene...Selective oxidation of 5-hydroxymethylfurfual(HMF) to 2,5-furandicarboxylic acid(FDCA) as a bioplastics monomer is efficiently promoted by a simple system without noble-metal and base additives. In this work, graphene oxide(GO) was first synthesised by an electrochemical method with flexible graphite paper(FGP) as start carbon material, then, nitrogen-doped graphene(NG) layers encapsulated Cu nanoparticles(NPs) was prepared by one-step thermal treatment of GO supported Cu2+ in flowing NH3 atmosphere. Compared with NG supported Cu NPs prepared by the traditional impregnation method, enhanced catalytic activity was achieved over Cu/NG and an FDCA yield of 95.2% was achieved under mild reaction conditions with tert-butylhydroperoxide(t-BuOOH) as the oxidant. Control experiments with different catalysts and different addition procedure of t-BuOOH showed the yield of HMF and various intermediates during reaction. From the changing of intermediates concentrations and reaction rates, a reaction pathway through HMF-DFF-FFCA-FDCA was proposed. This work gives a more convenient, more green,more economical and effective method in encapsulated metal NPs preparation and high selectivity in HMF oxidation to FDCA under mild conditions.展开更多
Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability cau...Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.展开更多
Alkaline seawater electrolysis for hydrogen production powered by clean energy is increasingly driving the development of a low-carbon economy.However,the limited proton availability in the electrolyte leads to sluggi...Alkaline seawater electrolysis for hydrogen production powered by clean energy is increasingly driving the development of a low-carbon economy.However,the limited proton availability in the electrolyte leads to sluggish cathodic reaction kinetics and elevates energy consumption,which hinders its large-scale application.Herein,low Pt loaded NiCo phosphate-coated NiCoP nanoneedle arrays on Ni foam(Pt@NCPi@NCP/NF)using a spontaneous redox strategy is developed for efficient and durable electrocatalytic hydrogen production from alkaline seawater.In situ Raman spectroscopy confirms that a large number of hydrated hydrogen ion intermediates are generated on the surface of Pt@NCPi@NCP/NF during the hydrogen evolution reaction(HER)process,which successfully constructs a localized acidic microenvironment.Concurrently,the surface Pi layer functions as a proton buffer layer,effectively regulating proton supply to enhance the utilization efficiency of active sites.As a result,the catalyst exhibits excellent HER kinetics under alkaline conditions with a Tafel slope of only 39.65 mV·dec^(-1)and a low overpotential of 136 mV to reach 1000 mA·cm^(-2).展开更多
Seawater electrolysis holds great promise for sustainable green hydrogen production,but it is challenged by chloride-induced corrosion.Herein,we demonstrate the hydrothermal preparation of Pb-doped NiFe layered double...Seawater electrolysis holds great promise for sustainable green hydrogen production,but it is challenged by chloride-induced corrosion.Herein,we demonstrate the hydrothermal preparation of Pb-doped NiFe layered double hydroxide on Ni foam(Pb-NiFe LDH/NF)for alkaline seawater oxidation electrocatalysis.Our Pb-NiFe LDH/NF requires a low overpotential of only 381 mV to attain a current density of 1000 mA·cm^(-2),superior to its NiFe LDH/NF counterpart(423 mV).Additionally,it operates continuously for 1000 h with negligible performance degradation and minimal active chlorine production.In situ Raman spectroscopy analysis reveals that Pb incorporation facilitates catalyst surface reconstruction,thereby enhancing oxygen evolution reaction activity.Importantly,Pb selectively adsorbs free Cl^(-)to form stable Pb-Cl species under the influence of an applied electric field.This process creates a Cl^(-)-free layer near the anode surface,thereby enhancing the catalyst’s chlorine corrosion resistance.展开更多
Background:The management of high complex anal fistulas has posed a significant challenge for surgeons.In this study,we presented a novel surgical procedure for managing high complex anal fistulas that combines core-o...Background:The management of high complex anal fistulas has posed a significant challenge for surgeons.In this study,we presented a novel surgical procedure for managing high complex anal fistulas that combines core-out fistulectomy with suture repair of the external anal sphincter defect and endorectal advancement flap.Methods:A cohort of patients with high complex anal fistulas undergoing core-out fistulectomy combined with suture repair of the external anal sphincter defect and endorectal advancement flap between December 2020 and December 2021 was reviewed retrospectively.Results:The median age of the patients was 43(range:25-53)years.All patients had high transsphincteric fistulas.Two of the five cases involved recurrent anal fistulas.During the median follow-up period of 23(range:23-34)months,no recurrence events were observed in the cohort.Furthermore,it was noted that no patients developed anal incontinence after the operation.Conclusion:Core-out fistulectomy combined with suture repair of the external anal sphincter defect and endorectal advancement flap is an effective procedure for the treatment of high complex anal fistulas.展开更多
The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reporte...The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reported as a highly active OER electrocatalyst in alkaline seawater,requiring only overpotentials of 303 and 332 mV to achieve 100 and 300 mA·cm^(-2),respectively.Moreover,it shows strong long-term electrochemical durability for at least 50 h.展开更多
Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited a...Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.展开更多
Introduction Rectovaginal fistula(RVF)presents with symptoms of passage of flatus or feces through the vagina,accompanied by severe sexual and psychosocial dysfunction in patients.For high-level RVF,the transabdominal...Introduction Rectovaginal fistula(RVF)presents with symptoms of passage of flatus or feces through the vagina,accompanied by severe sexual and psychosocial dysfunction in patients.For high-level RVF,the transabdominal approach represents the standard procedure[1,2].The management of RVF poses a considerable challenge for surgeons due to the relatively high recurrence rate.展开更多
Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the...Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the lifespan of seawater electrolysis systems.Herein,we present metal ion-chelated tannic acid nanoparticles anchored on the CoFe layered double hydroxide nanosheet array on nickel foam(CoFe LDH@CoFe-TA/NF),synthesized via an interfacial coordination assembly method,serving as an efficient and stable electrocatalyst for alkaline seawater oxidation(ASO).The formed CoFe-TA nanoparticles promote the transformation of Co^(3+)into the more robust acid Co^(4+),thereby favoring the adsorption of the hard base OH^(−)rather than the soft base Cl^(−).In addition,the CoFe-TA ligand network effectively inhibits metal ion leaching and stabilizes active sites.As a result,the CoFe LDH@CoFe-TA/NF electrode requires a low overpotential of only 379 mV to obtain a current density of 1000 mA cm^(−2)in 1 M KOH+seawater.Furthermore,the electrode also shows a stable operation for 450 h at an industrial-level current density,underscoring its potential for sustainable energy applications.展开更多
Renewable electricity-driven seawater electrolysis for hydrogen production offers substantial potential for sustainable energy solutions.However,the high concentration of chloride ions(Cl-)in seawater triggers competi...Renewable electricity-driven seawater electrolysis for hydrogen production offers substantial potential for sustainable energy solutions.However,the high concentration of chloride ions(Cl-)in seawater triggers competitive chemical reactions and severe corrosion,posing a challenge to the durability of the anode.In this study,we present a hexafluoroantimonate-intercalated NiFe layered double hydroxide nanosheet array on Ni foam(SbF_(6)^(-)-NiFe LDH/NF),which serves as a highly active and stable electrocatalyst for alkaline seawater oxidation(ASO).SbF_(6)^(-)-NiFe LDH/NF requires only an overpotential of 379 mV to achieve a current density of 1000 mA cm^(-2),significantly outperforming NiFe LDH/NF(396 mV).Furthermore,it exhibits excellent long-term stability over 600 hours at 1000 mA cm^(-2),with only trace amounts of active chlorine detected during the ASO process.In situ Raman spectroscopy confirms that the insertion of SbF_(6)^(-)into the LDH layers promotes the formation of active sites.More importantly,SbF_(6)^(-)efficiently repels Cl-,thus providing robust protection to the anode.This development represents a significant advancement in the design of noble-metal-free,durable anode electrodes for ASO.展开更多
基金the National Natural Science Foundation of China(NNSFC)(21805145&U1610108)the Department of Science and Technology of Shandong Province(ZR2019BB068)+2 种基金the Department of Science and Technology of Shanxi Province(201705D211001)Scientific and Technological Innovation Programs of High Education Institutions in Shanxi(201802001-1)the Department of Human Resource and Social Security of Shanxi Province(Y6SW9613B1)。
文摘Selective oxidation of 5-hydroxymethylfurfual(HMF) to 2,5-furandicarboxylic acid(FDCA) as a bioplastics monomer is efficiently promoted by a simple system without noble-metal and base additives. In this work, graphene oxide(GO) was first synthesised by an electrochemical method with flexible graphite paper(FGP) as start carbon material, then, nitrogen-doped graphene(NG) layers encapsulated Cu nanoparticles(NPs) was prepared by one-step thermal treatment of GO supported Cu2+ in flowing NH3 atmosphere. Compared with NG supported Cu NPs prepared by the traditional impregnation method, enhanced catalytic activity was achieved over Cu/NG and an FDCA yield of 95.2% was achieved under mild reaction conditions with tert-butylhydroperoxide(t-BuOOH) as the oxidant. Control experiments with different catalysts and different addition procedure of t-BuOOH showed the yield of HMF and various intermediates during reaction. From the changing of intermediates concentrations and reaction rates, a reaction pathway through HMF-DFF-FFCA-FDCA was proposed. This work gives a more convenient, more green,more economical and effective method in encapsulated metal NPs preparation and high selectivity in HMF oxidation to FDCA under mild conditions.
基金support from the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811)。
文摘Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.
文摘Alkaline seawater electrolysis for hydrogen production powered by clean energy is increasingly driving the development of a low-carbon economy.However,the limited proton availability in the electrolyte leads to sluggish cathodic reaction kinetics and elevates energy consumption,which hinders its large-scale application.Herein,low Pt loaded NiCo phosphate-coated NiCoP nanoneedle arrays on Ni foam(Pt@NCPi@NCP/NF)using a spontaneous redox strategy is developed for efficient and durable electrocatalytic hydrogen production from alkaline seawater.In situ Raman spectroscopy confirms that a large number of hydrated hydrogen ion intermediates are generated on the surface of Pt@NCPi@NCP/NF during the hydrogen evolution reaction(HER)process,which successfully constructs a localized acidic microenvironment.Concurrently,the surface Pi layer functions as a proton buffer layer,effectively regulating proton supply to enhance the utilization efficiency of active sites.As a result,the catalyst exhibits excellent HER kinetics under alkaline conditions with a Tafel slope of only 39.65 mV·dec^(-1)and a low overpotential of 136 mV to reach 1000 mA·cm^(-2).
基金funding this work through Large Research Project under Grant(No.RGP2/28/46).
文摘Seawater electrolysis holds great promise for sustainable green hydrogen production,but it is challenged by chloride-induced corrosion.Herein,we demonstrate the hydrothermal preparation of Pb-doped NiFe layered double hydroxide on Ni foam(Pb-NiFe LDH/NF)for alkaline seawater oxidation electrocatalysis.Our Pb-NiFe LDH/NF requires a low overpotential of only 381 mV to attain a current density of 1000 mA·cm^(-2),superior to its NiFe LDH/NF counterpart(423 mV).Additionally,it operates continuously for 1000 h with negligible performance degradation and minimal active chlorine production.In situ Raman spectroscopy analysis reveals that Pb incorporation facilitates catalyst surface reconstruction,thereby enhancing oxygen evolution reaction activity.Importantly,Pb selectively adsorbs free Cl^(-)to form stable Pb-Cl species under the influence of an applied electric field.This process creates a Cl^(-)-free layer near the anode surface,thereby enhancing the catalyst’s chlorine corrosion resistance.
基金supported by the Guangzhou Clinical High-Tech Project,Guangdong Province[grant number 2023P-GX09]The Sixth Affiliated Hospital,Sun Yat-sen University Clinical Research 1010 Program[grant number 1010PY(2020)-18]+1 种基金The Natural Science Foundation of Guangdong Province for Distinguished Young Scholars[grant number 2022B1515020003]National Key Clinical Discipline,Guangdong Provincial Clinical Research Center for Digestive Diseases[grant number 2020B1111170004].
文摘Background:The management of high complex anal fistulas has posed a significant challenge for surgeons.In this study,we presented a novel surgical procedure for managing high complex anal fistulas that combines core-out fistulectomy with suture repair of the external anal sphincter defect and endorectal advancement flap.Methods:A cohort of patients with high complex anal fistulas undergoing core-out fistulectomy combined with suture repair of the external anal sphincter defect and endorectal advancement flap between December 2020 and December 2021 was reviewed retrospectively.Results:The median age of the patients was 43(range:25-53)years.All patients had high transsphincteric fistulas.Two of the five cases involved recurrent anal fistulas.During the median follow-up period of 23(range:23-34)months,no recurrence events were observed in the cohort.Furthermore,it was noted that no patients developed anal incontinence after the operation.Conclusion:Core-out fistulectomy combined with suture repair of the external anal sphincter defect and endorectal advancement flap is an effective procedure for the treatment of high complex anal fistulas.
基金The authors extend their appreciation to the Deanship of Scientific Research at King Khalid University for funding support through large group Research Project(No.RGP2/257/44).
文摘The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reported as a highly active OER electrocatalyst in alkaline seawater,requiring only overpotentials of 303 and 332 mV to achieve 100 and 300 mA·cm^(-2),respectively.Moreover,it shows strong long-term electrochemical durability for at least 50 h.
基金supported by the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811).
文摘Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.
基金the Ethics Committee of Sun Yat-sen Hospital,Guangzhou,P.R.China(No.2023ZSLYEC-625).
文摘Introduction Rectovaginal fistula(RVF)presents with symptoms of passage of flatus or feces through the vagina,accompanied by severe sexual and psychosocial dysfunction in patients.For high-level RVF,the transabdominal approach represents the standard procedure[1,2].The management of RVF poses a considerable challenge for surgeons due to the relatively high recurrence rate.
基金the Deanship of Scientific Research at King Khalid University for funding support through a large group research project under Grant No.RGP2/119/45.
文摘Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the lifespan of seawater electrolysis systems.Herein,we present metal ion-chelated tannic acid nanoparticles anchored on the CoFe layered double hydroxide nanosheet array on nickel foam(CoFe LDH@CoFe-TA/NF),synthesized via an interfacial coordination assembly method,serving as an efficient and stable electrocatalyst for alkaline seawater oxidation(ASO).The formed CoFe-TA nanoparticles promote the transformation of Co^(3+)into the more robust acid Co^(4+),thereby favoring the adsorption of the hard base OH^(−)rather than the soft base Cl^(−).In addition,the CoFe-TA ligand network effectively inhibits metal ion leaching and stabilizes active sites.As a result,the CoFe LDH@CoFe-TA/NF electrode requires a low overpotential of only 379 mV to obtain a current density of 1000 mA cm^(−2)in 1 M KOH+seawater.Furthermore,the electrode also shows a stable operation for 450 h at an industrial-level current density,underscoring its potential for sustainable energy applications.
基金appreciation to the Deanship of Research and Graduate Studies at King Khalid University for funding this work through Large Research Project under Grant number RGP2/28/46.
文摘Renewable electricity-driven seawater electrolysis for hydrogen production offers substantial potential for sustainable energy solutions.However,the high concentration of chloride ions(Cl-)in seawater triggers competitive chemical reactions and severe corrosion,posing a challenge to the durability of the anode.In this study,we present a hexafluoroantimonate-intercalated NiFe layered double hydroxide nanosheet array on Ni foam(SbF_(6)^(-)-NiFe LDH/NF),which serves as a highly active and stable electrocatalyst for alkaline seawater oxidation(ASO).SbF_(6)^(-)-NiFe LDH/NF requires only an overpotential of 379 mV to achieve a current density of 1000 mA cm^(-2),significantly outperforming NiFe LDH/NF(396 mV).Furthermore,it exhibits excellent long-term stability over 600 hours at 1000 mA cm^(-2),with only trace amounts of active chlorine detected during the ASO process.In situ Raman spectroscopy confirms that the insertion of SbF_(6)^(-)into the LDH layers promotes the formation of active sites.More importantly,SbF_(6)^(-)efficiently repels Cl-,thus providing robust protection to the anode.This development represents a significant advancement in the design of noble-metal-free,durable anode electrodes for ASO.
