The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in s...The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.展开更多
Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to sta...Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to stabilize the Ir sites for effective OER.When anchored on the surface of Co_(3)O_(4)in the form of Ir(OH)_6 species,the created Ir-OH-Co interface leads to a limited stability and poor acidic OER due to Ir leaching.When doped into Co_(3)O_(4)lattice,the analyses of X-ray absorption spectroscopy,in-situ Raman,and OER measurements show that the partially replacement of Co in Co_(3)O_(4)by Ir atoms inclines to cause strong electronic effect and activate lattice oxygen in the presence of Ir-O-Co interface,and simultaneously master the reconstruction effect to mitigate Ir dissolution,realizing the improved OER activity and stability in alkaline and acidic environments.As a result,Ir_(lat)@Co_(3)O_(4)with Ir loading of 3.67 wt%requires 294±4 mV/285±3 mV and 326±2 mV to deliver 10 mA cm^(-2)in alkaline(0.1 M KOH/1.0 M KOH)and acidic(0.5 M H_(2)SO_(4))solution,respectively,with good stability.展开更多
The earth-abundant and high-performance catalysts are crucial for commercial implementation of hydrogen evolution reaction(HER).Herein,a multifunctional site strategy to construct excellent HER catalysts by incorporat...The earth-abundant and high-performance catalysts are crucial for commercial implementation of hydrogen evolution reaction(HER).Herein,a multifunctional site strategy to construct excellent HER catalysts by incorporating iridium(Ir)ions on the atomic scale into orthorhombic-CoSe2(Ir-CoSe_(2))was reported.Outstanding hydrogen evolution activity in alkaline media such as a low overpotential of 48.7 mV at a current density of 10 mA cm^(-2)and better performance than commercial Pt/C catalysts at high current densities were found in the Ir-CoSe_(2) samples.In the experiments and theoretical calculations,it was revealed that Ir enabled CoSe_(2)to form multifunctional sites to synergistically catalyze alkaline HER by promoting the adsorption and dissociation of H_(2)O(Ir sites)and optimizing the binding energy for H^(*)on Co sites.It was noticeable that the electrolytic system comprising the Ir-CoSe_(2)electrode not only produced hydrogen efficiently via HER,but also degraded organic pollutants(Methylene blue).The cell voltage of the dual-function electrolytic system was 1.58 V at the benchmark current density of 50 mA cm^(-2),which was significantly lower than the conventional water splitting voltage.It was indicated that this method was a novel strategy for designing advanced HER electrocatalysts by constructing multifunctional catalytic sites for hydrogen production and organic degradation.展开更多
The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To ad...The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.展开更多
Mussel aquaculture and large yellow croaker aquaculture areas and their environmental characteristics in Zhoushan were analyzed using satellite data and in-situ surveys.A new two-step remote sensing method was propose...Mussel aquaculture and large yellow croaker aquaculture areas and their environmental characteristics in Zhoushan were analyzed using satellite data and in-situ surveys.A new two-step remote sensing method was proposed and applied to determine the basic environmental characteristics of the best mussel and large yellow croaker aquaculture areas.This methodology includes the first step of extraction of the location distribution and the second step of the extraction of internal environmental factors.The fishery ranching index(FRI1,FRI2)was established to extract the mussel and the large yellow croaker aquaculture area in Zhoushan,using Gaofen-1(GF-1)and Gaofen-6(GF-6)satellite data with a special resolution of 2 m.In the second step,the environmental factors such as sea surface temperature(SST),chlorophyll a(Chl-a)concentration,current and tide,suspended sediment concentration(SSC)in mussel aquaculture area and large yellow croaker aquaculture area were extracted and analyzed in detail.The results show the following three points.(1)For the extraction of the mussel aquaculture area,FRI1 and FRI2 are complementary,and the combination of FRI1 and FRI2 is suitable to extract the mussel aquaculture area.As for the large yellow croaker aquaculture area extraction,FRI2 is suitable.(2)Mussel aquaculture and the large yellow croaker aquaculture area in Zhoushan are mainly located on the side near the islands that are away from the eastern open waters.The water environment factor template suitable for mussel and large yellow croaker aquaculture was determined.(3)This two-step remote sensing method can be used for the preliminary screening of potential site selection for the mussels and large yellow croaker aquaculture area in the future.the fishery ranching index(FRI1,FRI2)in this paper can be applied to extract the mussel and large yellow croaker aquaculture areas in coastal waters around the world.展开更多
Background: The optimal time to closure of a newborn with a myelomeningocele has been the focus of a number of evaluations. The Timing of primary surgery has received significant attention due to its relationship to r...Background: The optimal time to closure of a newborn with a myelomeningocele has been the focus of a number of evaluations. The Timing of primary surgery has received significant attention due to its relationship to repair-site infection that can lead to increased morbidity and prolonged hospital stays. It is on this basis that recommendations have utilized 48 - 72 hours post birth as ideal time of closure. This is not only prevent infection at the site but also prevent ventriculitis and neural structure damage. We therefore, hypothesized an increase in wound infection rates in those patients with delays in myelomeningocele repair. Methods: We retrospectively reviewed the records of 103 children with myelomeningocele treated between 2016 and 2023. At discharge the patients were followed up at the post-operative clinic visit 2 weeks later. Children were assigned to 1 of 2 groups, those who underwent primary neurosurgical repair within 72 hours of delivery (Group 1) and those undergoing repair after 72 hours (Group 2). We compared the infection rates. Results: 103 children who underwent myelomeningocele repair were identified, with a median time from birth to treatment of 1 day. Eight (7.8 %) patients were noted to have post-repair surgical site complications. There was no significant difference in rates of infection between Group 1 and Group 2 repair times. The presence of infection was associated increased length of stay when compared to neonates without infection. Conclusion: In children with myelomeningocele, the timing of primary neurosurgical repair appears not to have a significant impact on surgical site infection. Closure of the spinal lesion within the first 72 hours of life may be more favorable for neural damage prevention. These results suggest that early myelomeningocele repair may not impart significantly on the rate of wound-site infection.展开更多
On October 26,2022,the International Union of Geological Sciences(IUGS)unveiled the First 100 IUGS Geological Heritage Sites in Spain.These sites are located in56 countries,including 34 in the Americas,28 in Europe,15...On October 26,2022,the International Union of Geological Sciences(IUGS)unveiled the First 100 IUGS Geological Heritage Sites in Spain.These sites are located in56 countries,including 34 in the Americas,28 in Europe,15 in Africa and 23 in the Asia-Pacific-Middle East region(Table 1).The seven selected sites of China are introduced as follows(black font in Table 1).展开更多
BACKGROUND Despite the infrequency of trocar site hernias(TSHs),fascial closure continues to be recommended for their prevention when using a≥10-mm trocar.AIM To identify the necessity of fascial closure for a 12-mm ...BACKGROUND Despite the infrequency of trocar site hernias(TSHs),fascial closure continues to be recommended for their prevention when using a≥10-mm trocar.AIM To identify the necessity of fascial closure for a 12-mm nonbladed trocar incision in minimally invasive colorectal surgeries.METHODS Between July 2010 and December 2018,all patients who underwent minimally invasive colorectal surgery at the Minimally Invasive Surgery Unit of Siriraj Hospital were retrospectively reviewed.All patients underwent cross-sectional imaging for TSH assessment.Clinicopathological characteristics were recorded.Incidence rates of TSH and postoperative results were analyzed.RESULTS Of the 254 patients included,70(111 ports)were in the fascial closure(closed)group and 184(279 ports)were in the nonfascial closure(open)group.The median follow up duration was 43 mo.During follow up,three patients in the open group developed TSHs,whereas none in the closed group developed the condition(1.1%vs 0%,P=0.561).All TSHs occurred in the right lower abdomen.Patients whose drains were placed through the same incision had higher rates of TSHs compared with those without the drain.The open group had a significantly shorter operative time and lower blood loss than the closed group.CONCLUSION Routine performance of fascial closure when using a 12-mm nonbladed trocar may not be needed.However,further prospective studies with cross-sectional imaging follow-up and larger sample size are needed to confirm this finding.展开更多
The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs) attractive for oxygen electrocatalysis. The catalytic activities of DACs are largely decided by their surrou...The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs) attractive for oxygen electrocatalysis. The catalytic activities of DACs are largely decided by their surrounding micro-environment and supporting substrates. Modulating the micro-environment as well as engineering the efficient support is challenging tasks. Moreover, both are critical to optimizing the performance of DACs. Herein, a novel bio-cooperative strategy is developed to synthesize Fe Ni-DAC wherein Fe-Ni dual-atom sites are embedded in the N, P codoped tyre shaped carbon matrix. The configuration matching of Fe-Ni dual centers together with the local electronic engineering of N, P heteroatoms synergistically boost the catalytic activity on the oxygen reaction. Furthermore, the central-hollow highlyporous carbon matrix not only gives rise to a large amount of active sites, but also facilitates fast kinetics.Taking advantage of both the DAC and the substrate, the Fe Ni-NPC hollow tyre(HT) catalyst scores high in both oxygen reduction and evolution reactions, which exhibits the narrow potential difference and excellent durability. The aqueous Zn-air full battery(ZAB) integrating the Fe Ni-NPC HT air cathode has a high power density and a good stability over long-term cycling. Moreover, the flexible solid-state ZAB assembled with the polymer electrolyte obtains the high reliability over a wide range of temperatures or under diverse outside deformations. Therefore, this work offers a new green approach to prepare highly efficient DACs with built-in modulated micro-environment and tailor-made substrates. Moreover,it also paves a new way to develop highly-pliable power source for flexible electronics.展开更多
基金supported by the National Key Research and Development Program of China(2022YFB3807500)the Natural Science Foundation of China(22220102003)+3 种基金the Beijing Natural Science Foundation(JL23003)"Double-First-Class"construction projects(XK180301 and XK1804-02)China Postdoctoral Science Foundation 2023TQ0020Dostdoctoral Fellowship Program of CPSF(GZC20230199)。
文摘The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.
基金supported by the National Natural Science Foundation of China(52150410409).
文摘Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to stabilize the Ir sites for effective OER.When anchored on the surface of Co_(3)O_(4)in the form of Ir(OH)_6 species,the created Ir-OH-Co interface leads to a limited stability and poor acidic OER due to Ir leaching.When doped into Co_(3)O_(4)lattice,the analyses of X-ray absorption spectroscopy,in-situ Raman,and OER measurements show that the partially replacement of Co in Co_(3)O_(4)by Ir atoms inclines to cause strong electronic effect and activate lattice oxygen in the presence of Ir-O-Co interface,and simultaneously master the reconstruction effect to mitigate Ir dissolution,realizing the improved OER activity and stability in alkaline and acidic environments.As a result,Ir_(lat)@Co_(3)O_(4)with Ir loading of 3.67 wt%requires 294±4 mV/285±3 mV and 326±2 mV to deliver 10 mA cm^(-2)in alkaline(0.1 M KOH/1.0 M KOH)and acidic(0.5 M H_(2)SO_(4))solution,respectively,with good stability.
基金the financial support of the Doctoral Research Initiation Foundation of Linyi University(LYDX2020BS016)the National Natural Science Foundation of Shandong Province(ZR2021QB208,ZR2022MB054)+4 种基金the National Natural Science Foundation of China(22305262)SIAT Innovation Program for Excellent Young Researchers(2022)Shenzhen Science and Technology Program Grant(RCJC20200714114435061,ZDSYS20220527171406014)the City University of Hong Kong Donation Research Grants(9220061 and 9229021)City University of Hong Kong Strategic Research Grant(SRG 7005505)。
文摘The earth-abundant and high-performance catalysts are crucial for commercial implementation of hydrogen evolution reaction(HER).Herein,a multifunctional site strategy to construct excellent HER catalysts by incorporating iridium(Ir)ions on the atomic scale into orthorhombic-CoSe2(Ir-CoSe_(2))was reported.Outstanding hydrogen evolution activity in alkaline media such as a low overpotential of 48.7 mV at a current density of 10 mA cm^(-2)and better performance than commercial Pt/C catalysts at high current densities were found in the Ir-CoSe_(2) samples.In the experiments and theoretical calculations,it was revealed that Ir enabled CoSe_(2)to form multifunctional sites to synergistically catalyze alkaline HER by promoting the adsorption and dissociation of H_(2)O(Ir sites)and optimizing the binding energy for H^(*)on Co sites.It was noticeable that the electrolytic system comprising the Ir-CoSe_(2)electrode not only produced hydrogen efficiently via HER,but also degraded organic pollutants(Methylene blue).The cell voltage of the dual-function electrolytic system was 1.58 V at the benchmark current density of 50 mA cm^(-2),which was significantly lower than the conventional water splitting voltage.It was indicated that this method was a novel strategy for designing advanced HER electrocatalysts by constructing multifunctional catalytic sites for hydrogen production and organic degradation.
基金financially supported by the National Natural Science Foundation of China(21773024)the Natural Science Foundation of Sichuan Province of China(2023NSFC0084)the China Postdoctoral Science Foundation(2019M663469)。
文摘The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.
基金The National Key Research and Development Program of China under contract Nos 2023YFD2401900 and 2020YFD09008004the National Natural Science Foundation of China Key International(Regional)Cooperative Research Project under contract No.42020104009the Basic Public Welfare Research Program of Zhejiang Province under contract No.LGF21D010004.
文摘Mussel aquaculture and large yellow croaker aquaculture areas and their environmental characteristics in Zhoushan were analyzed using satellite data and in-situ surveys.A new two-step remote sensing method was proposed and applied to determine the basic environmental characteristics of the best mussel and large yellow croaker aquaculture areas.This methodology includes the first step of extraction of the location distribution and the second step of the extraction of internal environmental factors.The fishery ranching index(FRI1,FRI2)was established to extract the mussel and the large yellow croaker aquaculture area in Zhoushan,using Gaofen-1(GF-1)and Gaofen-6(GF-6)satellite data with a special resolution of 2 m.In the second step,the environmental factors such as sea surface temperature(SST),chlorophyll a(Chl-a)concentration,current and tide,suspended sediment concentration(SSC)in mussel aquaculture area and large yellow croaker aquaculture area were extracted and analyzed in detail.The results show the following three points.(1)For the extraction of the mussel aquaculture area,FRI1 and FRI2 are complementary,and the combination of FRI1 and FRI2 is suitable to extract the mussel aquaculture area.As for the large yellow croaker aquaculture area extraction,FRI2 is suitable.(2)Mussel aquaculture and the large yellow croaker aquaculture area in Zhoushan are mainly located on the side near the islands that are away from the eastern open waters.The water environment factor template suitable for mussel and large yellow croaker aquaculture was determined.(3)This two-step remote sensing method can be used for the preliminary screening of potential site selection for the mussels and large yellow croaker aquaculture area in the future.the fishery ranching index(FRI1,FRI2)in this paper can be applied to extract the mussel and large yellow croaker aquaculture areas in coastal waters around the world.
文摘Background: The optimal time to closure of a newborn with a myelomeningocele has been the focus of a number of evaluations. The Timing of primary surgery has received significant attention due to its relationship to repair-site infection that can lead to increased morbidity and prolonged hospital stays. It is on this basis that recommendations have utilized 48 - 72 hours post birth as ideal time of closure. This is not only prevent infection at the site but also prevent ventriculitis and neural structure damage. We therefore, hypothesized an increase in wound infection rates in those patients with delays in myelomeningocele repair. Methods: We retrospectively reviewed the records of 103 children with myelomeningocele treated between 2016 and 2023. At discharge the patients were followed up at the post-operative clinic visit 2 weeks later. Children were assigned to 1 of 2 groups, those who underwent primary neurosurgical repair within 72 hours of delivery (Group 1) and those undergoing repair after 72 hours (Group 2). We compared the infection rates. Results: 103 children who underwent myelomeningocele repair were identified, with a median time from birth to treatment of 1 day. Eight (7.8 %) patients were noted to have post-repair surgical site complications. There was no significant difference in rates of infection between Group 1 and Group 2 repair times. The presence of infection was associated increased length of stay when compared to neonates without infection. Conclusion: In children with myelomeningocele, the timing of primary neurosurgical repair appears not to have a significant impact on surgical site infection. Closure of the spinal lesion within the first 72 hours of life may be more favorable for neural damage prevention. These results suggest that early myelomeningocele repair may not impart significantly on the rate of wound-site infection.
文摘On October 26,2022,the International Union of Geological Sciences(IUGS)unveiled the First 100 IUGS Geological Heritage Sites in Spain.These sites are located in56 countries,including 34 in the Americas,28 in Europe,15 in Africa and 23 in the Asia-Pacific-Middle East region(Table 1).The seven selected sites of China are introduced as follows(black font in Table 1).
文摘BACKGROUND Despite the infrequency of trocar site hernias(TSHs),fascial closure continues to be recommended for their prevention when using a≥10-mm trocar.AIM To identify the necessity of fascial closure for a 12-mm nonbladed trocar incision in minimally invasive colorectal surgeries.METHODS Between July 2010 and December 2018,all patients who underwent minimally invasive colorectal surgery at the Minimally Invasive Surgery Unit of Siriraj Hospital were retrospectively reviewed.All patients underwent cross-sectional imaging for TSH assessment.Clinicopathological characteristics were recorded.Incidence rates of TSH and postoperative results were analyzed.RESULTS Of the 254 patients included,70(111 ports)were in the fascial closure(closed)group and 184(279 ports)were in the nonfascial closure(open)group.The median follow up duration was 43 mo.During follow up,three patients in the open group developed TSHs,whereas none in the closed group developed the condition(1.1%vs 0%,P=0.561).All TSHs occurred in the right lower abdomen.Patients whose drains were placed through the same incision had higher rates of TSHs compared with those without the drain.The open group had a significantly shorter operative time and lower blood loss than the closed group.CONCLUSION Routine performance of fascial closure when using a 12-mm nonbladed trocar may not be needed.However,further prospective studies with cross-sectional imaging follow-up and larger sample size are needed to confirm this finding.
基金supported by the Innovation Foundation of Graduate Student of Harbin Normal University (HSDSSCX2022-111)the Natural Science Foundation of Heilongjiang Province of China(TD2020B001)the Opening Project of State Key Laboratory of Advanced Chemical Power Sources (SKL-ACPS-C-25)。
文摘The electronic and functional synergies between the twin metal centers make dual single-atom catalysts(DACs) attractive for oxygen electrocatalysis. The catalytic activities of DACs are largely decided by their surrounding micro-environment and supporting substrates. Modulating the micro-environment as well as engineering the efficient support is challenging tasks. Moreover, both are critical to optimizing the performance of DACs. Herein, a novel bio-cooperative strategy is developed to synthesize Fe Ni-DAC wherein Fe-Ni dual-atom sites are embedded in the N, P codoped tyre shaped carbon matrix. The configuration matching of Fe-Ni dual centers together with the local electronic engineering of N, P heteroatoms synergistically boost the catalytic activity on the oxygen reaction. Furthermore, the central-hollow highlyporous carbon matrix not only gives rise to a large amount of active sites, but also facilitates fast kinetics.Taking advantage of both the DAC and the substrate, the Fe Ni-NPC hollow tyre(HT) catalyst scores high in both oxygen reduction and evolution reactions, which exhibits the narrow potential difference and excellent durability. The aqueous Zn-air full battery(ZAB) integrating the Fe Ni-NPC HT air cathode has a high power density and a good stability over long-term cycling. Moreover, the flexible solid-state ZAB assembled with the polymer electrolyte obtains the high reliability over a wide range of temperatures or under diverse outside deformations. Therefore, this work offers a new green approach to prepare highly efficient DACs with built-in modulated micro-environment and tailor-made substrates. Moreover,it also paves a new way to develop highly-pliable power source for flexible electronics.
