Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrat...Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic structure.It exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity.Specifically,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) pathway.This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.展开更多
Quercus arkansana(Arkansas oak)is at risk of becoming endangered,as the total known population size is represented by a few isolated populations.The potential impact of climate change on this species in the near futur...Quercus arkansana(Arkansas oak)is at risk of becoming endangered,as the total known population size is represented by a few isolated populations.The potential impact of climate change on this species in the near future is high,yet knowledge of its predicted effects is limited.Our study utilized the biomod2 R package to develop habi-tat suitability ensemble models based on bioclimatic and topographic environmental variables and the known loca-tions of current distribution of Q.arkansana.We predicted suitable habitats across three climate change scenarios(SSP1-2.6,SSP2-4.5,and SSP5-8.5)for 2050,2070,and 2090.Our findings reveal that the current suitable habitat for Q.arkansana is approximately 127,881 km^(2) across seven states(Texas,Arkansas,Alabama,Louisiana,Mississippi,Georgia,and Florida);approximately 9.5%is encompassed within state and federally managed protected areas.Our models predict that all current suitable habitats will disap-pear by 2050 due to climate change,resulting in a northward shift into new regions such as Tennessee and Kentucky.The large extent of suitable habitat outside protected areas sug-gests that a species-specific action plan incorporating pro-tected areas and other areas may be crucial for its conserva-tion.Moreover,protection of Q.arkansana habitat against climate change may require locally and regionally focused conservation policies,adaptive management strategies,and educational outreach among local people.展开更多
Understanding the physiological adaptations of non-treeline trees to environmental stress is important to understand future shifts in species composition and distribution of current treeline ecotone.The aim of the pre...Understanding the physiological adaptations of non-treeline trees to environmental stress is important to understand future shifts in species composition and distribution of current treeline ecotone.The aim of the present study was to elucidate the mechanisms of the formation of the upper elevation limit of non-treeline tree species,Picea jezoensis,and the carbon allocation strategies of the species on Changbai Mountain.We employed the^(13)C in situ pulse labeling technique to trace the distribution of photosynthetically assimilated carbon in Picea jezoensis at different elevational positions(tree species at its upper elevation limit(TSAUE,1,700 m a.s.l.)under treeline ecotone;tree species at a lower elevation position(TSALE,1,400 m a.s.l.).We analyzed^(13)C and the non-structural carbohydrate(NSC)concentrations in various tissues following labeling.Our findings revealed a significant shift in carbon allocation in TSAUE compared to TSALE.There was a pronounced increase inδ^(13)C allocation to belowground components(roots,soil,soil respiration)in TSAUE compared to TSALE.Furthermore,the C flow rate within the plant-soil-atmosphere system was faster,and the C residence time in the plant was shorter in TSAUE.The trends indicate enhanced C sink activity in belowground tissues in TSAUE,with newly assimilated C being preferentially directed there,suggesting a more conservative C allocation strategy by P.jezoensis at higher elevations under harsher environments.Such a strategy,prioritizing C storage in roots,likely aids in withstanding winter cold stress at the expense of aboveground growth during the growing season,leading to reduced growth of TSAUE compared to TSALE.The results of the present study shed light on the adaptive mechanisms governing the upper elevation limits of non-treeline trees,and enhances our understanding of how non-treeline species might respond to ongoing climate change.展开更多
Manganese oxide(MnO_(2))exhibits excellent activity for volatile organic compound oxidation.However,it is currently unknown whether lattice oxygen or adsorbed oxygen is more conducive to the progress of the catalytic ...Manganese oxide(MnO_(2))exhibits excellent activity for volatile organic compound oxidation.However,it is currently unknown whether lattice oxygen or adsorbed oxygen is more conducive to the progress of the catalytic reaction.In this study,novel hollow highly dispersed Pt/Copper modified-MnO_(2)catalysts were fabricated.Cu^(2+)was stabilized into theδ-MnO_(2)cladding substituting original K+,which produced lattice defects and enhance the content of adsorbed oxygen.The 2.03 wt%Pt Cu_(0.050)-MnO_(2)catalyst exhibited the highest catalytic activity and excellent stability for toluene and benzene oxidation,with T_(100)=160℃under high space velocity(36,000 mL g^(-1)h^(-1)).The excellent performance of catalytic oxidation of VOCs is attributed to the abundant adsorbed oxygen content,excellent low-temperature reducibility and the synergistic catalytic effect between the Pt nanoparticles and Cu_(0.050)-MnO_(2).This study provides a comprehensive understanding of the Langmuir-Hinshelwood(L-H)mechanism occurring on the catalysts.展开更多
In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally a...In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally accepted as the hydrogenating reactive species.This work for the first time proposed and confirmed the assisted catalytic mechanism of surface OH species that performed as the promoter for syngas-to-C_(2)species on Cu-based catalysts.DFT and microkinetic modeling results reveal that the produced OH species accompanying the intermediates CH_(x)production on the MCu(M=Co,Fe,Rh)catalysts can stably exist to form OH/MCu catalysts,on which the presence of surface OH species as the promoter not only presented better activity and selectivity toward CH_(x)(x=1-3)compared to MCu catalysts,but also significantly suppressed CH_(3)OH production,providing enough CH_(x)sources to favor the production of C_(2)hydrocarbons and oxygenates.Correspondingly,the electronic properties analysis revealed the essential relationship between the electronic feature of OH/MCu catalysts and catalytic performance,attributing to the unique electronic micro-environment of the catalysts under the interaction of surface OH species.This new mechanism is called as OH-assisted catalytic mechanism,which may be applied in the reaction systems related to the generation of OH species.展开更多
The Upper Guinea Forest is subject to heavy deforestation. In this context, many endemic and/or rare plant species are threatened with extinction. This is the case of Aubregrinia taïensis (Aubrév. & Pell...The Upper Guinea Forest is subject to heavy deforestation. In this context, many endemic and/or rare plant species are threatened with extinction. This is the case of Aubregrinia taïensis (Aubrév. & Pellegr.) Heine, a critically endangered Sapotaceae species, endemic to Côte d’Ivoire and Ghana. After 3 years of investigation in and around the Tai National Park (TNP) in the West of Côte d’Ivoire, only one individual of this species was located and no sexual reproductive organs (fruits, seeds) were observed. Woody plant species around this individual were inventoried in order to know the species that can co-occur with Aubregrinia taïensis. For that a plot of 30 m of diameter was established around the individual and all of the woody species of this circle were inventoried. Then, the taxonomic diversity, the chorology of the species, the conservation status and their life-form were recorded. A total of 130 woody plant species belonging to 51 families were collected in the site. The most represented families are Euphorbiaceae (12 spp.), Rubiaceae (10 spp.), Annonaceae (7 spp.), Fabaceae, Moraceae, Malvaceae (6 spp. each) while the most represented genera are Diospyros L. (4 spp.), Cola Schott & Endl. and Vitex L. (3 spp.). Species from the Guineo-Congolese Region (GC) are the most abundant (72%). They are followed by West African endemic species (GCW, 19%). Microphanerophytes (mp) are the most abundant and represent more than 40% of the species. Three vulnerable species were found in this plot: Campylospermum amplectens, Placodiscus boya and Trichoscypha cavalliensis. Thus, the preservation of this forest is more than necessary.展开更多
化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于...化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于光催化降解不同有机污染物显得尤为重要。采用一步无模板溶剂热法合成了核壳结构的C-TiO_(2)复合材料前驱体,并在氩气气氛下煅烧得到高结晶度的C-TiO_(2)复合光催化材料。运用SEM、TEM、XRD和TG等表征手段对材料进行表征,结论如下:550℃煅烧时的样品为包含少量碳的高结晶度的锐钛矿相TiO 2,且550℃煅烧时的样品依然保持了完整的核壳结构。此外,C-TiO_(2)复合材料的比表面积高达85.69 m 2·g^(-1),平均孔径为16.4 nm以及孔体积为0.423 m 3·g^(-1)。在UV-Vis光照射下,C-TiO_(2)复合材料分别对罗丹明B(RhB)、亚甲基蓝(MB)和刚果红(CR)3种染料显示出增强的光催化降解活性。展开更多
基金supported by the National Natural Science Foundation of China(Grant No.22072022)the Natural Science Foundation of Fujian Province(2021L3003)the Science Foundation of Shandong Province(ZR2019BB065).
文摘Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic structure.It exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity.Specifically,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) pathway.This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
基金The work was partially supported by research project funding from the Undergraduate Research Grant,Arkansas Tech University.
文摘Quercus arkansana(Arkansas oak)is at risk of becoming endangered,as the total known population size is represented by a few isolated populations.The potential impact of climate change on this species in the near future is high,yet knowledge of its predicted effects is limited.Our study utilized the biomod2 R package to develop habi-tat suitability ensemble models based on bioclimatic and topographic environmental variables and the known loca-tions of current distribution of Q.arkansana.We predicted suitable habitats across three climate change scenarios(SSP1-2.6,SSP2-4.5,and SSP5-8.5)for 2050,2070,and 2090.Our findings reveal that the current suitable habitat for Q.arkansana is approximately 127,881 km^(2) across seven states(Texas,Arkansas,Alabama,Louisiana,Mississippi,Georgia,and Florida);approximately 9.5%is encompassed within state and federally managed protected areas.Our models predict that all current suitable habitats will disap-pear by 2050 due to climate change,resulting in a northward shift into new regions such as Tennessee and Kentucky.The large extent of suitable habitat outside protected areas sug-gests that a species-specific action plan incorporating pro-tected areas and other areas may be crucial for its conserva-tion.Moreover,protection of Q.arkansana habitat against climate change may require locally and regionally focused conservation policies,adaptive management strategies,and educational outreach among local people.
基金supported by the National Natural Science Foundation of China(Grant numbers 4237105242271100+3 种基金4197112442371095)the Natural Science Foundation of Jilin Province,China(Nos.YDZJ202201ZYTS483YDZJ202201ZYTS470)。
文摘Understanding the physiological adaptations of non-treeline trees to environmental stress is important to understand future shifts in species composition and distribution of current treeline ecotone.The aim of the present study was to elucidate the mechanisms of the formation of the upper elevation limit of non-treeline tree species,Picea jezoensis,and the carbon allocation strategies of the species on Changbai Mountain.We employed the^(13)C in situ pulse labeling technique to trace the distribution of photosynthetically assimilated carbon in Picea jezoensis at different elevational positions(tree species at its upper elevation limit(TSAUE,1,700 m a.s.l.)under treeline ecotone;tree species at a lower elevation position(TSALE,1,400 m a.s.l.).We analyzed^(13)C and the non-structural carbohydrate(NSC)concentrations in various tissues following labeling.Our findings revealed a significant shift in carbon allocation in TSAUE compared to TSALE.There was a pronounced increase inδ^(13)C allocation to belowground components(roots,soil,soil respiration)in TSAUE compared to TSALE.Furthermore,the C flow rate within the plant-soil-atmosphere system was faster,and the C residence time in the plant was shorter in TSAUE.The trends indicate enhanced C sink activity in belowground tissues in TSAUE,with newly assimilated C being preferentially directed there,suggesting a more conservative C allocation strategy by P.jezoensis at higher elevations under harsher environments.Such a strategy,prioritizing C storage in roots,likely aids in withstanding winter cold stress at the expense of aboveground growth during the growing season,leading to reduced growth of TSAUE compared to TSALE.The results of the present study shed light on the adaptive mechanisms governing the upper elevation limits of non-treeline trees,and enhances our understanding of how non-treeline species might respond to ongoing climate change.
基金financial support provided by the National Key R&D Program of China(2020YFC1808401)National Natural Science Foundation of China(22078213,21938006,51973148,21776190)+1 种基金cuttingedge technology basic research project of Jiangsu(BK20202012)the project supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Manganese oxide(MnO_(2))exhibits excellent activity for volatile organic compound oxidation.However,it is currently unknown whether lattice oxygen or adsorbed oxygen is more conducive to the progress of the catalytic reaction.In this study,novel hollow highly dispersed Pt/Copper modified-MnO_(2)catalysts were fabricated.Cu^(2+)was stabilized into theδ-MnO_(2)cladding substituting original K+,which produced lattice defects and enhance the content of adsorbed oxygen.The 2.03 wt%Pt Cu_(0.050)-MnO_(2)catalyst exhibited the highest catalytic activity and excellent stability for toluene and benzene oxidation,with T_(100)=160℃under high space velocity(36,000 mL g^(-1)h^(-1)).The excellent performance of catalytic oxidation of VOCs is attributed to the abundant adsorbed oxygen content,excellent low-temperature reducibility and the synergistic catalytic effect between the Pt nanoparticles and Cu_(0.050)-MnO_(2).This study provides a comprehensive understanding of the Langmuir-Hinshelwood(L-H)mechanism occurring on the catalysts.
基金financially supported by Key Projects of National Natural Science Foundation of China(No.21736007)National Natural Science Foundation of China(Nos.22078221,21776193,21476155)Top Young Innovative Talents of Shanxi。
文摘In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally accepted as the hydrogenating reactive species.This work for the first time proposed and confirmed the assisted catalytic mechanism of surface OH species that performed as the promoter for syngas-to-C_(2)species on Cu-based catalysts.DFT and microkinetic modeling results reveal that the produced OH species accompanying the intermediates CH_(x)production on the MCu(M=Co,Fe,Rh)catalysts can stably exist to form OH/MCu catalysts,on which the presence of surface OH species as the promoter not only presented better activity and selectivity toward CH_(x)(x=1-3)compared to MCu catalysts,but also significantly suppressed CH_(3)OH production,providing enough CH_(x)sources to favor the production of C_(2)hydrocarbons and oxygenates.Correspondingly,the electronic properties analysis revealed the essential relationship between the electronic feature of OH/MCu catalysts and catalytic performance,attributing to the unique electronic micro-environment of the catalysts under the interaction of surface OH species.This new mechanism is called as OH-assisted catalytic mechanism,which may be applied in the reaction systems related to the generation of OH species.
文摘The Upper Guinea Forest is subject to heavy deforestation. In this context, many endemic and/or rare plant species are threatened with extinction. This is the case of Aubregrinia taïensis (Aubrév. & Pellegr.) Heine, a critically endangered Sapotaceae species, endemic to Côte d’Ivoire and Ghana. After 3 years of investigation in and around the Tai National Park (TNP) in the West of Côte d’Ivoire, only one individual of this species was located and no sexual reproductive organs (fruits, seeds) were observed. Woody plant species around this individual were inventoried in order to know the species that can co-occur with Aubregrinia taïensis. For that a plot of 30 m of diameter was established around the individual and all of the woody species of this circle were inventoried. Then, the taxonomic diversity, the chorology of the species, the conservation status and their life-form were recorded. A total of 130 woody plant species belonging to 51 families were collected in the site. The most represented families are Euphorbiaceae (12 spp.), Rubiaceae (10 spp.), Annonaceae (7 spp.), Fabaceae, Moraceae, Malvaceae (6 spp. each) while the most represented genera are Diospyros L. (4 spp.), Cola Schott & Endl. and Vitex L. (3 spp.). Species from the Guineo-Congolese Region (GC) are the most abundant (72%). They are followed by West African endemic species (GCW, 19%). Microphanerophytes (mp) are the most abundant and represent more than 40% of the species. Three vulnerable species were found in this plot: Campylospermum amplectens, Placodiscus boya and Trichoscypha cavalliensis. Thus, the preservation of this forest is more than necessary.
文摘化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于光催化降解不同有机污染物显得尤为重要。采用一步无模板溶剂热法合成了核壳结构的C-TiO_(2)复合材料前驱体,并在氩气气氛下煅烧得到高结晶度的C-TiO_(2)复合光催化材料。运用SEM、TEM、XRD和TG等表征手段对材料进行表征,结论如下:550℃煅烧时的样品为包含少量碳的高结晶度的锐钛矿相TiO 2,且550℃煅烧时的样品依然保持了完整的核壳结构。此外,C-TiO_(2)复合材料的比表面积高达85.69 m 2·g^(-1),平均孔径为16.4 nm以及孔体积为0.423 m 3·g^(-1)。在UV-Vis光照射下,C-TiO_(2)复合材料分别对罗丹明B(RhB)、亚甲基蓝(MB)和刚果红(CR)3种染料显示出增强的光催化降解活性。
