The development of facile strategies to tune the oxygen vacancy （OV） content in transition metal oxides （TMOs） is paramount to obtain low-cost and stable electrocatalysts, but still highly challenging. Taking NiC0...The development of facile strategies to tune the oxygen vacancy （OV） content in transition metal oxides （TMOs） is paramount to obtain low-cost and stable electrocatalysts, but still highly challenging. Taking NiC0204 as a model system, we have experimentally established a facile calcination and electrochemical activation （EA） methodology to dramatically increase the concentration of OVs and provide theoretical insight into how the concentration of OVs affects the performance of spinel TMOs towards the electrochemical hydrogen evolution reaction （HER）. A self-supported cathode of OV-rich NiC0204 nanowire arrays was found to exhibit higher HER activity and better stability in alkaline media than its counterparts with fewer OVs. The electrocatalytic HER activity was in good agreement with the increasing concentration of OVs in the studied samples. A large current density of 360 mA.cm-2 was reached with an overpotential of only 317 mV. Additionally, such a facile strategy was able to efficiently generate OVs in other TMOs （e.g., CoFe204 and NiFe204） for enhanced HER performance. In addition, our theoretical results suggest that the increasing OV concentration reduces the adsorption energy of water molecules and their dissociation energy barrier on the surface of the catalyst, thus leading to performance improvement of spinel TMOs toward the electrochemical HER. This work may open a new avenue to increase the concentration of OVs in TMOs in a controlled manner for promising applications in a variety of fields.展开更多
In some industrial plants, wastewater was intermittently or seasonally generated. There may be periods during which wastewater treatment facilities have to be set into an idle phase over several weeks. When wastewater...In some industrial plants, wastewater was intermittently or seasonally generated. There may be periods during which wastewater treatment facilities have to be set into an idle phase over several weeks. When wastewater was generated again, the activated sludge flocs may have disintegrated. In this experiment, re-activation characteristics of aerobic granular sludge starved for 2 months were investigated. Specific oxygen utilization rate(SOUR) was used as an indicator to evaluate the metabolic activity of the sludge. The results revealed that aerobic granular sludge could be stored up to two months without running the risk of losing the integrity of the granules and metabolic potentials. The apparent color of aerobic granules stored at room temperature gradually turned from brownish-yellowish to gray brown. They appeared brownish-yellowish again 2 weeks after re-activation. The velocity and strength of granules after 2-month idle period could be fully restored about 3 weeks after re-activation. Metabolic activity, however, dropped to 15 8 mg O_2/(g MLVSS·h), i.e. 74 % reduction after 2 months of storage. After restarting the reactor, it took 2 weeks that SOUR of up to 48 5 mg O_2 /(g MLVSS·h) was achieved. A stable effluent COD concentration of less than 150 mg/L was achieved during the re-activation process.展开更多
Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via ...Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via a precipitation-hydrothermal method by varying the amount of Ni during the precipitation step. The prepared nanosheets were subsequently used as supports for the deposition of Au nanoparticles(NPs). The obtained Au/Nix Al catalysts were studied in the context of CO oxidation to determine the effect of Ni doping on the supports. Enhanced catalytic performances were obtained for the Au/Nix Al catalysts compared with those of the Au supported on bare Al2 O3. The Ni content and pretreatment atmosphere were both shown to influence the catalytic activity. Pretreatment under a reducing atmosphere was beneficial for improving catalytic activity. The highest activity was observed for the catalysts with a Ni/Al molar ratio of 0.05, achieving complete CO conversion at 20 °C with a gold loading of 1 wt%. The in-situ FTIR results showed that the introduction of Ni strengthened CO adsorption on the Au NPs. The H2-TPR and O2-TPD results indicated that the introduction of Ni produced new oxygen vacancies and allowed the oxygen molecules to be adsorbed and activated more easily. The improved catalytic performance after doping Ni was attributed to the smaller size of the Au NPs and more active oxygen species.展开更多
Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Her...Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Herein,we propose a comprehensive strategy for the selective generation of reactive oxygen species(ROS)by regulating the sizes and facets of Au nanoparticles loaded on ZnO.For photocatalytic methane oxidation at ambient temperature,a high oxygenates yield of 36.4 mmol·g^(-1)·h^(-1) with a nearly 100%selectivity has been achieved over the optimized 1.0%Au/ZnO-9.6(1%Au with(111)facet and 9.6 nm size on ZnO)photocatalyst,exceeding most reported literatures.Mechanism investigations reveal that 1.0%Au/ZnO-9.6 with the medium size and Au(111)facet guarantees the favourable formation of superoxide radicals(·OOH)through mild oxygen reduction,ultimately leading to excellent photocatalytic methane oxidation performance.This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.展开更多
Though oxygen defects are associated with deteriorated structures and aggravated cycling performance in traditional layered cathodes,the role of oxygen defects is still ambiguous in Li-rich layered oxides due to the i...Though oxygen defects are associated with deteriorated structures and aggravated cycling performance in traditional layered cathodes,the role of oxygen defects is still ambiguous in Li-rich layered oxides due to the involvement of oxygen redox.Herein,a Co-free Li-rich layered oxide Li_(1.286)Ni_(0.071)Mn_(0.643)O_(2)has been prepared by a co-precipitation method to systematically investigate the undefined effects of the oxygen defects.A significant O_(2)release and the propagation of oxygen vacancies were detected by operando differential electrochemical mass spectroscopy(DEMS)and electron energy loss spectroscopy(EELS),respectively.Scanning transmission electron microscopy-high angle annular dark field(STEMHAADF)reveals the oxygen vacancies fusing to nanovoids and monitors a stepwise electrochemical activation process of the large Li_(2)MnO_(3)domain upon cycling.Combined with the quantitative analysis conducted by the energy dispersive spectrometer(EDS),existed nano-scale oxygen defects actually expose more surface to the electrolyte for facilitating the electrochemical activation and subsequently increasing available capacity.Overall,this work persuasively elucidates the function of oxygen defects on oxygen redox in Co-free Li-rich layered oxides.展开更多
Piezoelectric semiconductors bear the bifunctional photocatalysis and piezocatalysis,while the absent or weak internal charge driving force severely restricts its catalytic activity.Developing polarization strategy is...Piezoelectric semiconductors bear the bifunctional photocatalysis and piezocatalysis,while the absent or weak internal charge driving force severely restricts its catalytic activity.Developing polarization strategy is desirable,and particularly understanding its mechanism from a microscopic perspective remains scanty.Herein,we report a secondary recrystallization approach to achieving the simultaneous micro-and macroscopic polarization enhancement on Bi2WO6 nanosheets for boosting piezo-photocatalytic oxygen activation,and unravel the mechanism at an atom-level.The secondary recrystallization process not only results in a strengthened distortion of[WO6]octahedra with distortion index enhancement by~20%for a single octahedron,but also enables lateral crystal growth of nanosheets along the ab plane(av.50 to 180 nm),which separately allows the rise in dipole moment of unit cell(e.g.,1.63 D increase along a axis)and the stacking of the distorted[WO6]octahedron to accumulate the unit cell dipole,collectively contributing to the considerably strengthened spontaneous polarization and piezoelectricity.Besides,exposure of large-area{001}front facet enables more efficient capture and conversion of stress into piezo-potential.Therefore,the well-recrystallized Bi2WO6 nanosheets exhibit considerably promoted piezo-photocatalytic reactive oxygen species generation,given the decreased specific surface area.This work presents a feasible methodology to regulate inside-out polarization for guiding carriers transfer behavior,and may advance the solid understanding on the intrinsic mechanism.展开更多
To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3...To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3)catalysts were prepared.The characteristics of the catalysts showed that Mn reduced the crystallinity of the active CuO component,increased the number of oxygen vacancies and acidic sites on the catalyst surface,enhanced the mobility of surface oxygen,and the interaction between copper and manganese promoted the redox cycling ability of the catalysts and improved their oxidation performance,which increased the conversion frequency(TOF)by 2.54×10^(-2)to 3.07×10^(-2)sec^(-1).On the other hand,the introduction of Mn reduced the production of phosphate and As_(2)O_(3)on the catalyst surface by30.96%and 44.9%,which reduced the coverage and inerting of the active sites by phosphate and As_(2)O_(3),resulting in an 8 hr(6 hr)improvement in the stability of PH_(3)(AsH_(3))removal.展开更多
The function-led design of porous hydrochar from mineral-rich biowaste for environmental applications inevitably suffers from carbon-ash recalcitrance.However,a method to alter the original carbon skeleton with ash re...The function-led design of porous hydrochar from mineral-rich biowaste for environmental applications inevitably suffers from carbon-ash recalcitrance.However,a method to alter the original carbon skeleton with ash remains elusive and hinders the availability of hydrochar.Herein,we propose a facile strategy for breaking the rigid structure of carbon-ash coupled hydrochar using phase-tunable molten carbonates.A case system was designed in which livestock manure and NaHCO3 were used to prepare the activated hydrochar,and NH3 served as the target contaminant.Due to the redox effect,we found that organic fractions significantly advanced the melting temperature of Na2CO3 below 800℃.The Na species steadily broke the carbon-ash interaction as the thermal intensity increased and transformed inorganic constituents to facilitate ash dissolution,rebuilding the hydrochar skeleton with abundant hierarchical channels and active defect edges.The surface polarity and mesopore distribution collectively governed the five cycles NH3 adsorption attenuation process.Manure hydrochar delivered favorable potential for application with a maximum overall adsorption capacity of 100.49 mg·g^(-1).Integrated spectroscopic characterization and theoretical computations revealed that incorporating NH3 on the carbon surface could transfer electrons to chemisorbed oxygen,which promoted the oxidation of pyridine-N during adsorption.This work offers deep insight into the structure function correlation of hydrochar and inspires a more rational design of engineered hydrochar from high-ash biowaste.展开更多
Dehydrogenation is considered as one of the most important industrial applications for renewable energy.Cubic ceria-based catalysts are known to display promising dehydrogenation performances in this area.Large partic...Dehydrogenation is considered as one of the most important industrial applications for renewable energy.Cubic ceria-based catalysts are known to display promising dehydrogenation performances in this area.Large particle size(>20 nm)and less surface defects,however,hinder further application of ceria materials.Herein,an alternative strategy involving lactic acid(LA)assisted hydrothermal method was developed to synthesize active,selective and durable cubic ceria of<6 nm for dehydrogenation reactions.Detailed studies of growth mechanism revealed that,the carboxyl and hydroxyl groups in LA molecule synergistically manipulate the morphological evolution of ceria precursors.Carboxyl groups determine the cubic shape and particle size,while hydroxyl groups promote compositional transformation of ceria precursors into CeO_(2) phases.Moreover,enhanced oxygen vacancies(Vo)on the surface of CeO_(2) were obtained owing to continuous removal of O species under reductive atmosphere.Cubic CeO_(2) catalysts synthesized by the LA-assisted method,immobilized with bimetallic PtCo clusters,exhibit a record high activity(TOF:29,241 h^(-1))and Vo-dependent synergism for dehydrogenation of bio-derived polyols at 200℃.We also found that quenching Vo defects at air atmosphere causes activity loss of PtCo/CeO_(2) catalysts.To regenerate Vo defects,a simple strategy was developed by irradiating deactivated catalysts using hernia lamp.The outcome of this work will provide new insights into manufacturing durable catalyst materials for aqueous phase dehydrogenation applications.展开更多
文摘The development of facile strategies to tune the oxygen vacancy （OV） content in transition metal oxides （TMOs） is paramount to obtain low-cost and stable electrocatalysts, but still highly challenging. Taking NiC0204 as a model system, we have experimentally established a facile calcination and electrochemical activation （EA） methodology to dramatically increase the concentration of OVs and provide theoretical insight into how the concentration of OVs affects the performance of spinel TMOs towards the electrochemical hydrogen evolution reaction （HER）. A self-supported cathode of OV-rich NiC0204 nanowire arrays was found to exhibit higher HER activity and better stability in alkaline media than its counterparts with fewer OVs. The electrocatalytic HER activity was in good agreement with the increasing concentration of OVs in the studied samples. A large current density of 360 mA.cm-2 was reached with an overpotential of only 317 mV. Additionally, such a facile strategy was able to efficiently generate OVs in other TMOs （e.g., CoFe204 and NiFe204） for enhanced HER performance. In addition, our theoretical results suggest that the increasing OV concentration reduces the adsorption energy of water molecules and their dissociation energy barrier on the surface of the catalyst, thus leading to performance improvement of spinel TMOs toward the electrochemical HER. This work may open a new avenue to increase the concentration of OVs in TMOs in a controlled manner for promising applications in a variety of fields.
文摘In some industrial plants, wastewater was intermittently or seasonally generated. There may be periods during which wastewater treatment facilities have to be set into an idle phase over several weeks. When wastewater was generated again, the activated sludge flocs may have disintegrated. In this experiment, re-activation characteristics of aerobic granular sludge starved for 2 months were investigated. Specific oxygen utilization rate(SOUR) was used as an indicator to evaluate the metabolic activity of the sludge. The results revealed that aerobic granular sludge could be stored up to two months without running the risk of losing the integrity of the granules and metabolic potentials. The apparent color of aerobic granules stored at room temperature gradually turned from brownish-yellowish to gray brown. They appeared brownish-yellowish again 2 weeks after re-activation. The velocity and strength of granules after 2-month idle period could be fully restored about 3 weeks after re-activation. Metabolic activity, however, dropped to 15 8 mg O_2/(g MLVSS·h), i.e. 74 % reduction after 2 months of storage. After restarting the reactor, it took 2 weeks that SOUR of up to 48 5 mg O_2 /(g MLVSS·h) was achieved. A stable effluent COD concentration of less than 150 mg/L was achieved during the re-activation process.
文摘Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via a precipitation-hydrothermal method by varying the amount of Ni during the precipitation step. The prepared nanosheets were subsequently used as supports for the deposition of Au nanoparticles(NPs). The obtained Au/Nix Al catalysts were studied in the context of CO oxidation to determine the effect of Ni doping on the supports. Enhanced catalytic performances were obtained for the Au/Nix Al catalysts compared with those of the Au supported on bare Al2 O3. The Ni content and pretreatment atmosphere were both shown to influence the catalytic activity. Pretreatment under a reducing atmosphere was beneficial for improving catalytic activity. The highest activity was observed for the catalysts with a Ni/Al molar ratio of 0.05, achieving complete CO conversion at 20 °C with a gold loading of 1 wt%. The in-situ FTIR results showed that the introduction of Ni strengthened CO adsorption on the Au NPs. The H2-TPR and O2-TPD results indicated that the introduction of Ni produced new oxygen vacancies and allowed the oxygen molecules to be adsorbed and activated more easily. The improved catalytic performance after doping Ni was attributed to the smaller size of the Au NPs and more active oxygen species.
基金supported by the National Key Research and Development Program of China(No.2019YFA0708700)the National Natural Science Foundation of China(Nos.22322815,22179146,51672309,51172285,51372277)+5 种基金the Major Scientific and Technological Innovation Project of Shandong Province(No.2020CXGC010402)the Fundamental Research Funds for Central Universities(No.18CX07009A)YanKuang Group Co.,Ltd.(No.YKZB2020-167)the Young Taishan Scholar Program of Shandong Province(No.tsqn20182027)Taishan Scholar Project(No.ts201712020)the Technological Leading Scholar of 10000 Talent Project(No.W03020508).
文摘Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Herein,we propose a comprehensive strategy for the selective generation of reactive oxygen species(ROS)by regulating the sizes and facets of Au nanoparticles loaded on ZnO.For photocatalytic methane oxidation at ambient temperature,a high oxygenates yield of 36.4 mmol·g^(-1)·h^(-1) with a nearly 100%selectivity has been achieved over the optimized 1.0%Au/ZnO-9.6(1%Au with(111)facet and 9.6 nm size on ZnO)photocatalyst,exceeding most reported literatures.Mechanism investigations reveal that 1.0%Au/ZnO-9.6 with the medium size and Au(111)facet guarantees the favourable formation of superoxide radicals(·OOH)through mild oxygen reduction,ultimately leading to excellent photocatalytic methane oxidation performance.This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.
基金supported by the National Natural Science Foundation of China(52272253)the"Lingyan"Research and Development Plan of Zhejiang Province(2022C01071)+2 种基金the S&T Innovation 2025 Major Special Programme of Ningbo(2018B10081)the Natural Science Foundation of Ningbo(202003N4030)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2022299)。
文摘Though oxygen defects are associated with deteriorated structures and aggravated cycling performance in traditional layered cathodes,the role of oxygen defects is still ambiguous in Li-rich layered oxides due to the involvement of oxygen redox.Herein,a Co-free Li-rich layered oxide Li_(1.286)Ni_(0.071)Mn_(0.643)O_(2)has been prepared by a co-precipitation method to systematically investigate the undefined effects of the oxygen defects.A significant O_(2)release and the propagation of oxygen vacancies were detected by operando differential electrochemical mass spectroscopy(DEMS)and electron energy loss spectroscopy(EELS),respectively.Scanning transmission electron microscopy-high angle annular dark field(STEMHAADF)reveals the oxygen vacancies fusing to nanovoids and monitors a stepwise electrochemical activation process of the large Li_(2)MnO_(3)domain upon cycling.Combined with the quantitative analysis conducted by the energy dispersive spectrometer(EDS),existed nano-scale oxygen defects actually expose more surface to the electrolyte for facilitating the electrochemical activation and subsequently increasing available capacity.Overall,this work persuasively elucidates the function of oxygen defects on oxygen redox in Co-free Li-rich layered oxides.
基金the National Key Research and Development Program of China(No.2022YFB3803600)the National Natural Science Foundation of China(Nos.52272244 and 51972288)+1 种基金the Fundamental Research Funds for the Central Universities(No.2652022202)2021 Graduate Innovation Fund Project of China University of Geosciences,Beijing(No.ZY2021YC006).
文摘Piezoelectric semiconductors bear the bifunctional photocatalysis and piezocatalysis,while the absent or weak internal charge driving force severely restricts its catalytic activity.Developing polarization strategy is desirable,and particularly understanding its mechanism from a microscopic perspective remains scanty.Herein,we report a secondary recrystallization approach to achieving the simultaneous micro-and macroscopic polarization enhancement on Bi2WO6 nanosheets for boosting piezo-photocatalytic oxygen activation,and unravel the mechanism at an atom-level.The secondary recrystallization process not only results in a strengthened distortion of[WO6]octahedra with distortion index enhancement by~20%for a single octahedron,but also enables lateral crystal growth of nanosheets along the ab plane(av.50 to 180 nm),which separately allows the rise in dipole moment of unit cell(e.g.,1.63 D increase along a axis)and the stacking of the distorted[WO6]octahedron to accumulate the unit cell dipole,collectively contributing to the considerably strengthened spontaneous polarization and piezoelectricity.Besides,exposure of large-area{001}front facet enables more efficient capture and conversion of stress into piezo-potential.Therefore,the well-recrystallized Bi2WO6 nanosheets exhibit considerably promoted piezo-photocatalytic reactive oxygen species generation,given the decreased specific surface area.This work presents a feasible methodology to regulate inside-out polarization for guiding carriers transfer behavior,and may advance the solid understanding on the intrinsic mechanism.
基金supported by the National Natural Science Foundation of China (Nos.51868030,52070090,52100122,22266019,and 21876071)the Science and Technology Planning Project of Yunnan Province (Nos.202001AU070031,202101BE070001-030,and 202101BC070001-009)Applied Basic Research Program of Yunnan Province (No.2019FD043)。
文摘To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3)catalysts were prepared.The characteristics of the catalysts showed that Mn reduced the crystallinity of the active CuO component,increased the number of oxygen vacancies and acidic sites on the catalyst surface,enhanced the mobility of surface oxygen,and the interaction between copper and manganese promoted the redox cycling ability of the catalysts and improved their oxidation performance,which increased the conversion frequency(TOF)by 2.54×10^(-2)to 3.07×10^(-2)sec^(-1).On the other hand,the introduction of Mn reduced the production of phosphate and As_(2)O_(3)on the catalyst surface by30.96%and 44.9%,which reduced the coverage and inerting of the active sites by phosphate and As_(2)O_(3),resulting in an 8 hr(6 hr)improvement in the stability of PH_(3)(AsH_(3))removal.
基金supported by the National Natural Science Foundation of China(52261145701 and U21A20162)the 2115 Talent Development Program of China Agricultural University.
文摘The function-led design of porous hydrochar from mineral-rich biowaste for environmental applications inevitably suffers from carbon-ash recalcitrance.However,a method to alter the original carbon skeleton with ash remains elusive and hinders the availability of hydrochar.Herein,we propose a facile strategy for breaking the rigid structure of carbon-ash coupled hydrochar using phase-tunable molten carbonates.A case system was designed in which livestock manure and NaHCO3 were used to prepare the activated hydrochar,and NH3 served as the target contaminant.Due to the redox effect,we found that organic fractions significantly advanced the melting temperature of Na2CO3 below 800℃.The Na species steadily broke the carbon-ash interaction as the thermal intensity increased and transformed inorganic constituents to facilitate ash dissolution,rebuilding the hydrochar skeleton with abundant hierarchical channels and active defect edges.The surface polarity and mesopore distribution collectively governed the five cycles NH3 adsorption attenuation process.Manure hydrochar delivered favorable potential for application with a maximum overall adsorption capacity of 100.49 mg·g^(-1).Integrated spectroscopic characterization and theoretical computations revealed that incorporating NH3 on the carbon surface could transfer electrons to chemisorbed oxygen,which promoted the oxidation of pyridine-N during adsorption.This work offers deep insight into the structure function correlation of hydrochar and inspires a more rational design of engineered hydrochar from high-ash biowaste.
基金financial supports National Natural Science Foundation of China(22078365,21706290)Natural Science Foundation of Shandong Province(ZR2017MB004)+2 种基金Innovative Research Funding from Qingdao City,Shandong Province(17-1-1-80-jch)“Fundamental Research Funds for the Central Universities”and“the Development Fund of State Key Laboratory of Heavy Oil Processing”(17CX02017A,20CX02204A)Postgraduate Innovation Project(YCX2021057)from China University of Petroleum.
文摘Dehydrogenation is considered as one of the most important industrial applications for renewable energy.Cubic ceria-based catalysts are known to display promising dehydrogenation performances in this area.Large particle size(>20 nm)and less surface defects,however,hinder further application of ceria materials.Herein,an alternative strategy involving lactic acid(LA)assisted hydrothermal method was developed to synthesize active,selective and durable cubic ceria of<6 nm for dehydrogenation reactions.Detailed studies of growth mechanism revealed that,the carboxyl and hydroxyl groups in LA molecule synergistically manipulate the morphological evolution of ceria precursors.Carboxyl groups determine the cubic shape and particle size,while hydroxyl groups promote compositional transformation of ceria precursors into CeO_(2) phases.Moreover,enhanced oxygen vacancies(Vo)on the surface of CeO_(2) were obtained owing to continuous removal of O species under reductive atmosphere.Cubic CeO_(2) catalysts synthesized by the LA-assisted method,immobilized with bimetallic PtCo clusters,exhibit a record high activity(TOF:29,241 h^(-1))and Vo-dependent synergism for dehydrogenation of bio-derived polyols at 200℃.We also found that quenching Vo defects at air atmosphere causes activity loss of PtCo/CeO_(2) catalysts.To regenerate Vo defects,a simple strategy was developed by irradiating deactivated catalysts using hernia lamp.The outcome of this work will provide new insights into manufacturing durable catalyst materials for aqueous phase dehydrogenation applications.
