Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv...Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.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
Tree radial growth can have significantly differ-ent responses to climate change depending on the environ-ment.To elucidate the effects of climate on radial growth and stable carbon isotope(δ^(13)C)fractionation of Q...Tree radial growth can have significantly differ-ent responses to climate change depending on the environ-ment.To elucidate the effects of climate on radial growth and stable carbon isotope(δ^(13)C)fractionation of Qing-hai spruce(Picea crassifolia),a widely distributed native conifer in northwestern China in different environments,we developed chronologies for tree-ring widths and δ^(13)C in trees on the southern and northern slopes of the Qilian Mountains,and analysed the relationship between these tree-ring variables and major climatic factors.Tree-ring widths were strongly influenced by climatic factors early in the growing season,and the radial growth in trees on the northern slopes was more sensitive to climate than in trees on the southern.Tree-ring δ^(13)C was more sensitive to climate than radial growth.δ^(13)C fractionation was mainly influenced by summer temperature and precipitation early in the growing season.Stomatal conductance more strongly limited stable carbon isotope fractionation in tree rings than photosynthetic rate did.The response between tree rings and climate in mountains gradually weakened as climate warmed.Changes in radial growth and stable carbon isotope fractionation of P.crassifolia in response to climate in the Qilian Mountains may be further complicated by continued climate change.展开更多
Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a...Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.展开更多
Carbon(C),nitrogen(N),and phosphorus(P)are of fundamental importance for growth and nutrient dynamics within plant organs and deserve more attention at regional to global scales.However,our knowledge of how these nutr...Carbon(C),nitrogen(N),and phosphorus(P)are of fundamental importance for growth and nutrient dynamics within plant organs and deserve more attention at regional to global scales.However,our knowledge of how these nutrients vary with tree size,organ age,or root order at the individual level remains limited.We determined C,N,and P contents and their stoichiometric ratios(i.e.,nutrient traits)in needles,branches,and fine roots at different organ ages(0-3-year-old needles and branches)and root orders(1st-4th order roots)from 64 Pinus koraiensis of varying size(Diameter at breast height ranged from 0.3 to 100 cm)in northeast China.Soil factors were also measured.The results show that nutrient traits were regulated by tree size,organ age,or root order rather than soil factors.At a whole-plant level,nutrient traits decreased in needles and fine roots but increased in branches with tree size.At the organ level,age or root order had a negative effect on C,N,and P and a positive effect on stoichiometric ratios.Our results demonstrate that nutrient variations are closely related to organ-specific functions and ecophysiological processes at an individual level.It is suggested that the nutrient acquisition strategy by younger trees and organ fractions with higher nutrient content is for survival.Conversely,nutrient storage strategy in older trees and organ fractions are mainly for steady growth.Our results clarified the nutrient utilization strategies during tree and organ ontogeny and suggest that tree size and organ age or root order should be simultaneously considered to understand the complexities of nutrient variations.展开更多
BACKGROUND C23,an oligo-peptide derived from cold-inducible RNA-binding protein(CIRP),has been reported to inhibit tissue inflammation,apoptosis and fibrosis by binding to the CIRP receptor;however,there are few repor...BACKGROUND C23,an oligo-peptide derived from cold-inducible RNA-binding protein(CIRP),has been reported to inhibit tissue inflammation,apoptosis and fibrosis by binding to the CIRP receptor;however,there are few reports on its role in liver fibrosis and the underlying mechanism is unknown.AIM To explore whether C23 plays a significant role in carbon tetrachloride(CCl4)-induced liver fibrosis.METHODS CCl4 was injected for 6 weeks to induce liver fibrosis and C23 was used beginning in the second week.Masson and Sirius red staining were used to examine changes in fiber levels.Inflammatory factors in the liver were detected and changes inα-smooth muscle actin(α-SMA)and collagen I expression were detected via immu-nohistochemical staining to evaluate the activation of hematopoietic stellate cells(HSCs).Western blotting was used to detect the activation status of the trans-forming growth factor-beta(TGF-β)/Smad3 axis after C23 treatment.RESULTS CCl4 successfully induced liver fibrosis in mice,while tumor necrosis factor-alpha(TNF-α),IL(interleukin)-1β,and IL-6 levels increased significantly and the IL-10 level decreased significantly.Interestingly,C23 inhibited this process.On the other hand,C23 significantly inhibited the activation of HSCs induced by CCl4,which inhibited the expression ofα-SMA and the synthesis of collagen I.In terms of mechanism,C23 can block Smad3 phosphorylation significantly and inhibits INTRODUCTION At present there is no specific and effective drug for treating liver fibrosis caused by acute or chronic injury.Although preclinical research has made breakthroughs,their suitability as clinical treatments is still unknown.The activation of hepatic stellate cells(HSCs)caused by chronic inflammation is a key process in the development of liver fibrosis and activated HSCs expressα-smooth muscle actin(α-SMA)and transdifferentiate into myofibroblasts with proliferation,migration and secretion abilities,synthesizing the extracellular matrix to deposit in the hepatocyte space and subse-quently forming liver fibrosis[1].Although therapeutic strategies have improved due to past few efforts there is no ideal treatment for hepatic fibrosis[2].Extracellular cold inducible RNA binding protein(CIRP)has been shown to play a role in various acute and chronic inflammatory diseases by promoting tissue inflammation and apoptosis and inducing fibrosis through its receptor Toll-like receptor 4(TLR4)[3].C23 is a recognized competitive inhibitor of CIRP that can competitively bind to CIRP receptors and reduce tissue damage in inflammatory diseases[4].C23 has been shown to significantly reduce serum tumor necrosis factor-alpha(TNF-α),IL(interleukin)-6 and IL-1βlevels.In addition,it can reduce tissue TLR4,TNF-α,IL-6 and IL-1βlevels and inhibit the colocalization of CIRP and TLR4,which plays a significant role in systemic inflammation[5].Re-search has shown that CIRP induces the inflammatory phenotype of lung fibroblasts in a TLR4-dependent manner[6].On the other hand,CIRP is associated with markers of fibrosis andα-SMA is significantly positively correlated with CIRP.Cirp-/-mice exhibit attenuated expression ofα-SMA and collagen(COL1A1 and COL3A1),decreased hydroxyproline content,decreased histological fibrosis scores,and improved pulmonary hypertension[7].C23 inhibited the release of TNF-α,the degradation of IκB and the nuclear translocation of NF-κB in CIRP-stimulated macrophages in a dose-dependent manner and C23 treatment significantly increased the serum levels of lactic dehydrogenase,alanine ami-notransferase,IL-6,TNF-αand IL-1βin septic CLP mice[8].Based on previous research we hypothesized that C23 might alleviate liver fibrosis by inhibiting acute and chronic inflammation.As a selective hepatotoxic chemical carbon tetrachloride(CCl4).can induce inflammation and activate HSCs,promoting liver fibrosis.This study reveals the role and mechanism of C23 in CCl4-induced liver fibrosis in mice.at room temperature for 30 minutes.The gray value of each group was calculated after chemiluminescence.展开更多
Soil salinization is a critical environmental issue restricting agricultural production.Deep return of straw to the soil as an interlayer (at 40 cm depth) has been a popular practice to alleviate salt stress.However,t...Soil salinization is a critical environmental issue restricting agricultural production.Deep return of straw to the soil as an interlayer (at 40 cm depth) has been a popular practice to alleviate salt stress.However,the legacy effects of straw added as an interlayer at different rates on soil organic carbon (SOC) and total nitrogen (TN) in saline soils still remain inconclusive.Therefore,a four-year (2015–2018) field experiment was conducted with four levels (i.e.,0,6,12and 18 Mg ha~(–1)) of straw returned as an interlayer.Compared with no straw interlayer (CK),straw addition increased SOC concentration by 14–32 and 11–57%in the 20–40 and 40–60 cm soil layers,respectively.The increases in soil TN concentration (8–22 and 6–34%in the 20–40 and 40–60 cm soil layers,respectively) were lower than that for SOC concentration,which led to increased soil C:N ratio in the 20–60 cm soil depth.Increases in SOC and TN concentrations in the 20–60 cm soil layer with straw addition led to a decrease in stratification ratios (0–20 cm:20–60 cm),which promoted uniform distributions of SOC and TN in the soil profile.Increases in SOC and TN concentrations were associated with soil salinity and moisture regulation and improved sunflower yield.Generally,compared with other treatments,the application of 12 Mg ha~(–1) straw had higher SOC,TN and C:N ratio,and lower soil stratification ratio in the2015–2017 period.The results highlighted that legacy effects of straw application as an interlayer were maintained for at least four years,and demonstrated that deep soil straw application had a great potential for improving subsoil fertility in salt-affected soils.展开更多
Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,...Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing challenges.Here,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 products.The resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V vs.RHE(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_x.This strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and kinetically.The intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x electrocatalyst.This work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.展开更多
Soil samples were collected from different rubber fields in twenty-five plotsselected randomly in the Experimental Farm of the Chinese Academy of Tropical Agriculture Scienceslocated in Hainan, China, to analyse the e...Soil samples were collected from different rubber fields in twenty-five plotsselected randomly in the Experimental Farm of the Chinese Academy of Tropical Agriculture Scienceslocated in Hainan, China, to analyse the ecological effect of rubber cultivation. The results showedthat in the tropical rubber farm, soil microbial biomass C (MBC) and total organic C (TOC) wererelatively low in the content but highly correlated with each other. After rubber tapping, soil MBCof mature rubber fields decreased significantly, by 55.5 percent. compared with immature rubberfields. Soil TOC also decreased but the difference was not significant. Ratios of MBC to TOCdecreased significantly. The decreasing trend of MBC stopped at about ten years of rubbercultivation. After this period, soil MBC increased relatively while soil TOC still kept indecreasing. Soil MBC changes could be measured to predict the tendency of soil organic matterchanges due to management practices in a tropical rubber farm several years before the changes insoil TOC become detectable.展开更多
Soil organic carbon and nitrogen are used as indexes of soil quality assessment and sustainable land use management. At the same time, soil C/N ratio is a sensitive indicator of soil quality and for assessing the carb...Soil organic carbon and nitrogen are used as indexes of soil quality assessment and sustainable land use management. At the same time, soil C/N ratio is a sensitive indicator of soil quality and for assessing the carbon and nitrogen nutrition balance of soils. We studied the characteristics of soil organic carbon and total nitrogen by investigating a large number of apple orchards in major apple production areas in China. High apple orchard soil organic carbon content was observed in the provinces of Heilongjiang, Xinjiang, and Yunnan, whereas low content was found in the provinces of Shandong, Henan, Hebei, and Shaanxi, with the values ranging between 6.44 and 7.76 g·kg-1. Similar to soil organic carbon, soil total nitrogen content also exhibited obvious differences in the 12 major apple producing provinces. Shandong apple orchard soil had the highest total nitrogen content (1.26 g·kg-1), followed by Beijing (1.23 g·kg-1). No significant difference was noted between these two regions, but their total nitrogen content was significantly higher than the other nine provinces, excluding Yunnan. The soil total nitrogen content for Xinjiang, Heilongjiang, Hebei, Henan, and Gansu was between 0.87 and 1.03 g·kg-1, which was significantly lower than that in Shandong and Beijing, but significantly higher than that in Liaoning, Shanxi, and Shaanxi. Six provinces exhibited apple orchard soil C/N ratio higher than 10, including Heilongjiang (15.42), Xinjiang (13.38), Ningxia (14.45), Liaoning (12.24), Yunnan (11.03), and Gansu (10.63). The soil C/N ratio was below 10 in the remaining six provinces, in which the highest was found in Shaanxi (9.47), followed by Beijing (8.98), Henan (7.99), and Shanxi (7.62), and the lowest was found in Hebei (6.80) and Shandong (6.05). Therefore, the improvement of soil organic carbon should be given more attention to increase the steady growth of soil C/N ratio.展开更多
Soil organic carbon(SOC)and its stable isotope composition reflect key information about the carbon cycle in ecosystems.Studies of carbon fractions in oasis continuous cotton-cropped fields can elucidate the SOC stabi...Soil organic carbon(SOC)and its stable isotope composition reflect key information about the carbon cycle in ecosystems.Studies of carbon fractions in oasis continuous cotton-cropped fields can elucidate the SOC stability mechanism under the action of the human-land relationship during the oasification of arid land,which is critical for understanding the carbon dynamics of terrestrial ecosystems in arid lands under global climate change.In this study,we investigated the Alar Reclamation Area on the northern edge of the Tarim Basin,Xinjiang Uygur Autonomous Region of China,in 2020.In original desert and oasis farmlands with different reclamation years,including 6,10,18,and 30 a,and different soil depths(0-20,20-40,40-60 cm),we analyzed the variations in SOC,very liable carbon(C_(VL)),liable carbon(C_(L)),less liable carbon(C_(LL)),and non-liable carbon(C_(NL))using the method of spatial series.The differences in the stable carbon isotope ratio(δ^(13)C)and beta(β)values reflecting the organic carbon decomposition rate were also determined during oasification.Through redundancy analysis,we derived and discussed the relationships among SOC,carbon fractions,δ^(13)C,and other soil physicochemical properties,such as the soil water content(SWC),bulk density(BD),pH,total salt(TS),total nitrogen(TN),available phosphorus(AP),and available potassium(AK).The results showed that there were significant differences in SOC and carbon fractions of oasis farmlands with different reclamation years,and the highest SOC was observed at the oasis farmland with 30-a reclamation year.C_(VL),C_(L),C_(LL),and C_(NL) showed significant changes among oasis farmlands with different reclamation years,and C_(VL) had the largest variation range(0.40-4.92 g/kg)and accounted for the largest proportion in the organic carbon pool.The proportion of C_(NL) in the organic carbon pool of the topsoil(0-20 cm)gradually increased.δ^(13)C varied from-25.61‰to-22.58‰,with the topsoil showing the most positive value at the oasis farmland with 10-a reclamation year;while theβvalue was the lowest at the oasis farmland with 6-a reclamation year and then increased significantly.Based on the redundancy analysis results,the soil physicochemical properties,such as TN,AP,AK,and pH,were significantly correlated with C_(L),and TN and AP were positively correlated with C_(VL).However,δ^(13)C was not significantly influenced by soil physicochemical properties.Our analysis advances the understanding of SOC dynamics during oasification,revealing the risk of soil carbon loss and its contribution to terrestrial carbon accumulation in arid lands,which could be useful for the sustainable development of regional carbon resources and ecological protection in arid ecosystem.展开更多
Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenera...Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenerated charge carries and photocatalyzed organic reactions for the conversion of solar energy into chemical energy. Herein, we deposited well-dispersed Pd NPs with small size on crystallized carbon nitride(CN–C) to construct a Schottky-type Pd/CN–C hybrid for photocatalyzed Ullmann C–C homocoupling of aryl halides under visible light irradiation at room temperature. Compared to Pd NPs supported g-C_3N_4(Pd/g-C_3N_4), Pd/CN–C exhibits excellent visible light photocatalytic activity for Ullmann C–C coupling of aryl halides due to high crystallinity of CN–C support, high dispersion and smaller size of Pd NPs, and the interfacial heterojunction of Pd/CN–C. Upon visible light irradiation, more photogenerated electrons from CN–C flow across the Schottky junction to metallic Pd and trigger the Ullmann C–C coupling of aryl halides. The photogenerated holes on CN–C surface are captured by a protic solvent(such as EtOH). In the presence of base K_2CO_3, the solvent undergoes dissociation, dehydrogenation, and finally can be oxidized by captured photogenerated holes. Moreover, Pd/CN–C has general applicability for various substrates and shows excellent stability and reusability for more than nine cycles.展开更多
The processing of an energy carrier such as microalgae oil into valuable fuels and chemicals is quite promising.Aqueous-phase processing is suitable for this purpose because the separation of intrinsic water from the ...The processing of an energy carrier such as microalgae oil into valuable fuels and chemicals is quite promising.Aqueous-phase processing is suitable for this purpose because the separation of intrinsic water from the algae cell is difficult.In this study,we synthesized ruthenium(Ru)nanoparticles supported on highly hydrophilic mesoporous carbon to catalyze the quantitative hydrodeoxygenation(HDO)of microalgae oil to alkanes in a one-pot process at a low temperature(140℃)in the aqueous phase.The mesoporous carbon was obtained by single-step calcination of starch and zinc chloride in nitrogen.The as-obtained carbon showed high surface areas and pore volumes,allowing high dispersion of Ru nanoparticles.The surface of the carbon material was rich in hydroxyl groups,as evidenced by X-ray photoelectron spectroscopy(XPS),infrared(IR)spectroscopy,and thermogravimetric analysis(TGA)measurements.As a result,the carbon material contacted preferably with the water phase versus the organic phase,improving the accessibility of substrates.On the other hand,the contact angle test results speculated the superior hydrophilic nature of mesoporous Ru/C(ZnCl2,starch)than commercial Ru/C.Both kinetics modeling and in situ IR monitoring in water revealed the superior performance of the hydrophilic mesoporous and hydrophilic Ru/C compared to a commercial Ru/C for the tandem hydrogenation of stearic acid and decarbonylation of stearyl alcohol.The herein designed hydrothermal carbon material was highly active,environmentally benign,sustainable,and recyclable material,and could be potentially used for other hydrogenation reactions in the aqueous phase.展开更多
基金financially supported by the National Natural Science Foundation of China (22372001)Starting Fund for Scientific Research of High-Level Talents, Anhui Agricultural University (rc382108)+1 种基金Anhui Provincial Key Research and Development Plan (2022e07020037)Innovation and Entrepreneurship Training Program for College Students (X202310364204, S202210364046, X202310364209)
文摘Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.
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supported by Basic Research Operating Expenses of the Central level Non-profit Research Institutes (IDM2022003)National Natural Science Foundation of China (42375054)+2 种基金Regional collaborative innovation project of Xinjiang (2021E01022,2022E01045)Young Meteorological Talent Program of China Meteorological Administration,Tianshan Talent Program of Xinjiang (2022TSYCCX0003)Youth Innovation Team of China Meteorological Administration (CMA2023QN08).
文摘Tree radial growth can have significantly differ-ent responses to climate change depending on the environ-ment.To elucidate the effects of climate on radial growth and stable carbon isotope(δ^(13)C)fractionation of Qing-hai spruce(Picea crassifolia),a widely distributed native conifer in northwestern China in different environments,we developed chronologies for tree-ring widths and δ^(13)C in trees on the southern and northern slopes of the Qilian Mountains,and analysed the relationship between these tree-ring variables and major climatic factors.Tree-ring widths were strongly influenced by climatic factors early in the growing season,and the radial growth in trees on the northern slopes was more sensitive to climate than in trees on the southern.Tree-ring δ^(13)C was more sensitive to climate than radial growth.δ^(13)C fractionation was mainly influenced by summer temperature and precipitation early in the growing season.Stomatal conductance more strongly limited stable carbon isotope fractionation in tree rings than photosynthetic rate did.The response between tree rings and climate in mountains gradually weakened as climate warmed.Changes in radial growth and stable carbon isotope fractionation of P.crassifolia in response to climate in the Qilian Mountains may be further complicated by continued climate change.
基金the National Natural Science Foundation of China(51303083)the National Natural Science Foundation of China for Excellent Young Scholars(51922050)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20191293)the Fundamental Research Funds for the Central Universities(30920021123)。
文摘Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.
基金supported by the National Key R&D Program of China (2022YFD2201100)Natural Science Foundation of Heilongjiang Province of China (TD2023C006)the Fundamental Research Funds for the Central Universities (2572022DS13).
文摘Carbon(C),nitrogen(N),and phosphorus(P)are of fundamental importance for growth and nutrient dynamics within plant organs and deserve more attention at regional to global scales.However,our knowledge of how these nutrients vary with tree size,organ age,or root order at the individual level remains limited.We determined C,N,and P contents and their stoichiometric ratios(i.e.,nutrient traits)in needles,branches,and fine roots at different organ ages(0-3-year-old needles and branches)and root orders(1st-4th order roots)from 64 Pinus koraiensis of varying size(Diameter at breast height ranged from 0.3 to 100 cm)in northeast China.Soil factors were also measured.The results show that nutrient traits were regulated by tree size,organ age,or root order rather than soil factors.At a whole-plant level,nutrient traits decreased in needles and fine roots but increased in branches with tree size.At the organ level,age or root order had a negative effect on C,N,and P and a positive effect on stoichiometric ratios.Our results demonstrate that nutrient variations are closely related to organ-specific functions and ecophysiological processes at an individual level.It is suggested that the nutrient acquisition strategy by younger trees and organ fractions with higher nutrient content is for survival.Conversely,nutrient storage strategy in older trees and organ fractions are mainly for steady growth.Our results clarified the nutrient utilization strategies during tree and organ ontogeny and suggest that tree size and organ age or root order should be simultaneously considered to understand the complexities of nutrient variations.
基金Supported by The Panzhihua Science and Technology Planning Project of China,No.2023ZD-S-57.
文摘BACKGROUND C23,an oligo-peptide derived from cold-inducible RNA-binding protein(CIRP),has been reported to inhibit tissue inflammation,apoptosis and fibrosis by binding to the CIRP receptor;however,there are few reports on its role in liver fibrosis and the underlying mechanism is unknown.AIM To explore whether C23 plays a significant role in carbon tetrachloride(CCl4)-induced liver fibrosis.METHODS CCl4 was injected for 6 weeks to induce liver fibrosis and C23 was used beginning in the second week.Masson and Sirius red staining were used to examine changes in fiber levels.Inflammatory factors in the liver were detected and changes inα-smooth muscle actin(α-SMA)and collagen I expression were detected via immu-nohistochemical staining to evaluate the activation of hematopoietic stellate cells(HSCs).Western blotting was used to detect the activation status of the trans-forming growth factor-beta(TGF-β)/Smad3 axis after C23 treatment.RESULTS CCl4 successfully induced liver fibrosis in mice,while tumor necrosis factor-alpha(TNF-α),IL(interleukin)-1β,and IL-6 levels increased significantly and the IL-10 level decreased significantly.Interestingly,C23 inhibited this process.On the other hand,C23 significantly inhibited the activation of HSCs induced by CCl4,which inhibited the expression ofα-SMA and the synthesis of collagen I.In terms of mechanism,C23 can block Smad3 phosphorylation significantly and inhibits INTRODUCTION At present there is no specific and effective drug for treating liver fibrosis caused by acute or chronic injury.Although preclinical research has made breakthroughs,their suitability as clinical treatments is still unknown.The activation of hepatic stellate cells(HSCs)caused by chronic inflammation is a key process in the development of liver fibrosis and activated HSCs expressα-smooth muscle actin(α-SMA)and transdifferentiate into myofibroblasts with proliferation,migration and secretion abilities,synthesizing the extracellular matrix to deposit in the hepatocyte space and subse-quently forming liver fibrosis[1].Although therapeutic strategies have improved due to past few efforts there is no ideal treatment for hepatic fibrosis[2].Extracellular cold inducible RNA binding protein(CIRP)has been shown to play a role in various acute and chronic inflammatory diseases by promoting tissue inflammation and apoptosis and inducing fibrosis through its receptor Toll-like receptor 4(TLR4)[3].C23 is a recognized competitive inhibitor of CIRP that can competitively bind to CIRP receptors and reduce tissue damage in inflammatory diseases[4].C23 has been shown to significantly reduce serum tumor necrosis factor-alpha(TNF-α),IL(interleukin)-6 and IL-1βlevels.In addition,it can reduce tissue TLR4,TNF-α,IL-6 and IL-1βlevels and inhibit the colocalization of CIRP and TLR4,which plays a significant role in systemic inflammation[5].Re-search has shown that CIRP induces the inflammatory phenotype of lung fibroblasts in a TLR4-dependent manner[6].On the other hand,CIRP is associated with markers of fibrosis andα-SMA is significantly positively correlated with CIRP.Cirp-/-mice exhibit attenuated expression ofα-SMA and collagen(COL1A1 and COL3A1),decreased hydroxyproline content,decreased histological fibrosis scores,and improved pulmonary hypertension[7].C23 inhibited the release of TNF-α,the degradation of IκB and the nuclear translocation of NF-κB in CIRP-stimulated macrophages in a dose-dependent manner and C23 treatment significantly increased the serum levels of lactic dehydrogenase,alanine ami-notransferase,IL-6,TNF-αand IL-1βin septic CLP mice[8].Based on previous research we hypothesized that C23 might alleviate liver fibrosis by inhibiting acute and chronic inflammation.As a selective hepatotoxic chemical carbon tetrachloride(CCl4).can induce inflammation and activate HSCs,promoting liver fibrosis.This study reveals the role and mechanism of C23 in CCl4-induced liver fibrosis in mice.at room temperature for 30 minutes.The gray value of each group was calculated after chemiluminescence.
基金funded by the National Natural Science Foundation of China (31871584)the Agricultural Science and Technology Innovation Program, Chinese Academy of Agricultural Sciences (CAAS-ZDRW202201)+2 种基金the Fundamental Research Funds for Central Non-profit Scientific Institution, China (1610132020011)the “Open the list” in charge of the Science and Technology Project of Ordos, Center for Agro-pastoral Ecology and Resource Conservation of Ordos City, Inner Mongolia, China (JBGS2021-001)the Inner Mongolia Autonomous Region Research Project (2021EEDSCXSFQZD011)。
文摘Soil salinization is a critical environmental issue restricting agricultural production.Deep return of straw to the soil as an interlayer (at 40 cm depth) has been a popular practice to alleviate salt stress.However,the legacy effects of straw added as an interlayer at different rates on soil organic carbon (SOC) and total nitrogen (TN) in saline soils still remain inconclusive.Therefore,a four-year (2015–2018) field experiment was conducted with four levels (i.e.,0,6,12and 18 Mg ha~(–1)) of straw returned as an interlayer.Compared with no straw interlayer (CK),straw addition increased SOC concentration by 14–32 and 11–57%in the 20–40 and 40–60 cm soil layers,respectively.The increases in soil TN concentration (8–22 and 6–34%in the 20–40 and 40–60 cm soil layers,respectively) were lower than that for SOC concentration,which led to increased soil C:N ratio in the 20–60 cm soil depth.Increases in SOC and TN concentrations in the 20–60 cm soil layer with straw addition led to a decrease in stratification ratios (0–20 cm:20–60 cm),which promoted uniform distributions of SOC and TN in the soil profile.Increases in SOC and TN concentrations were associated with soil salinity and moisture regulation and improved sunflower yield.Generally,compared with other treatments,the application of 12 Mg ha~(–1) straw had higher SOC,TN and C:N ratio,and lower soil stratification ratio in the2015–2017 period.The results highlighted that legacy effects of straw application as an interlayer were maintained for at least four years,and demonstrated that deep soil straw application had a great potential for improving subsoil fertility in salt-affected soils.
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
基金the National Natural Science Foundation of China (21902017)the Foundation of technological innovation and application development of Chongqing (cstc2021jscxmsxm X0308, CSTB2022BSXM-JCX0132)+1 种基金the Youth project of science and technology research program of Chongqing Education Commission of China (KJQN20211107)the Scientific Research Foundation of Chongqing University of Technology (2020ZDZ022, 2021PYZ13)。
文摘Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing challenges.Here,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 products.The resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V vs.RHE(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_x.This strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and kinetically.The intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x electrocatalyst.This work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.
基金Project supported by the National Key Basic Research Support Foundation of China (No. G1999011809)the United Nations Development Programme (UNDP, No. CPR/96/105).
文摘Soil samples were collected from different rubber fields in twenty-five plotsselected randomly in the Experimental Farm of the Chinese Academy of Tropical Agriculture Scienceslocated in Hainan, China, to analyse the ecological effect of rubber cultivation. The results showedthat in the tropical rubber farm, soil microbial biomass C (MBC) and total organic C (TOC) wererelatively low in the content but highly correlated with each other. After rubber tapping, soil MBCof mature rubber fields decreased significantly, by 55.5 percent. compared with immature rubberfields. Soil TOC also decreased but the difference was not significant. Ratios of MBC to TOCdecreased significantly. The decreasing trend of MBC stopped at about ten years of rubbercultivation. After this period, soil MBC increased relatively while soil TOC still kept indecreasing. Soil MBC changes could be measured to predict the tendency of soil organic matterchanges due to management practices in a tropical rubber farm several years before the changes insoil TOC become detectable.
文摘Soil organic carbon and nitrogen are used as indexes of soil quality assessment and sustainable land use management. At the same time, soil C/N ratio is a sensitive indicator of soil quality and for assessing the carbon and nitrogen nutrition balance of soils. We studied the characteristics of soil organic carbon and total nitrogen by investigating a large number of apple orchards in major apple production areas in China. High apple orchard soil organic carbon content was observed in the provinces of Heilongjiang, Xinjiang, and Yunnan, whereas low content was found in the provinces of Shandong, Henan, Hebei, and Shaanxi, with the values ranging between 6.44 and 7.76 g·kg-1. Similar to soil organic carbon, soil total nitrogen content also exhibited obvious differences in the 12 major apple producing provinces. Shandong apple orchard soil had the highest total nitrogen content (1.26 g·kg-1), followed by Beijing (1.23 g·kg-1). No significant difference was noted between these two regions, but their total nitrogen content was significantly higher than the other nine provinces, excluding Yunnan. The soil total nitrogen content for Xinjiang, Heilongjiang, Hebei, Henan, and Gansu was between 0.87 and 1.03 g·kg-1, which was significantly lower than that in Shandong and Beijing, but significantly higher than that in Liaoning, Shanxi, and Shaanxi. Six provinces exhibited apple orchard soil C/N ratio higher than 10, including Heilongjiang (15.42), Xinjiang (13.38), Ningxia (14.45), Liaoning (12.24), Yunnan (11.03), and Gansu (10.63). The soil C/N ratio was below 10 in the remaining six provinces, in which the highest was found in Shaanxi (9.47), followed by Beijing (8.98), Henan (7.99), and Shanxi (7.62), and the lowest was found in Hebei (6.80) and Shandong (6.05). Therefore, the improvement of soil organic carbon should be given more attention to increase the steady growth of soil C/N ratio.
基金supported by the Scientific Research Program of the Higher Education Institution of Xinjiang(XJEDU2021I1005).
文摘Soil organic carbon(SOC)and its stable isotope composition reflect key information about the carbon cycle in ecosystems.Studies of carbon fractions in oasis continuous cotton-cropped fields can elucidate the SOC stability mechanism under the action of the human-land relationship during the oasification of arid land,which is critical for understanding the carbon dynamics of terrestrial ecosystems in arid lands under global climate change.In this study,we investigated the Alar Reclamation Area on the northern edge of the Tarim Basin,Xinjiang Uygur Autonomous Region of China,in 2020.In original desert and oasis farmlands with different reclamation years,including 6,10,18,and 30 a,and different soil depths(0-20,20-40,40-60 cm),we analyzed the variations in SOC,very liable carbon(C_(VL)),liable carbon(C_(L)),less liable carbon(C_(LL)),and non-liable carbon(C_(NL))using the method of spatial series.The differences in the stable carbon isotope ratio(δ^(13)C)and beta(β)values reflecting the organic carbon decomposition rate were also determined during oasification.Through redundancy analysis,we derived and discussed the relationships among SOC,carbon fractions,δ^(13)C,and other soil physicochemical properties,such as the soil water content(SWC),bulk density(BD),pH,total salt(TS),total nitrogen(TN),available phosphorus(AP),and available potassium(AK).The results showed that there were significant differences in SOC and carbon fractions of oasis farmlands with different reclamation years,and the highest SOC was observed at the oasis farmland with 30-a reclamation year.C_(VL),C_(L),C_(LL),and C_(NL) showed significant changes among oasis farmlands with different reclamation years,and C_(VL) had the largest variation range(0.40-4.92 g/kg)and accounted for the largest proportion in the organic carbon pool.The proportion of C_(NL) in the organic carbon pool of the topsoil(0-20 cm)gradually increased.δ^(13)C varied from-25.61‰to-22.58‰,with the topsoil showing the most positive value at the oasis farmland with 10-a reclamation year;while theβvalue was the lowest at the oasis farmland with 6-a reclamation year and then increased significantly.Based on the redundancy analysis results,the soil physicochemical properties,such as TN,AP,AK,and pH,were significantly correlated with C_(L),and TN and AP were positively correlated with C_(VL).However,δ^(13)C was not significantly influenced by soil physicochemical properties.Our analysis advances the understanding of SOC dynamics during oasification,revealing the risk of soil carbon loss and its contribution to terrestrial carbon accumulation in arid lands,which could be useful for the sustainable development of regional carbon resources and ecological protection in arid ecosystem.
基金financially supported by the National Natural Science Foundation of China(No.21503127)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2017JM2008)the 111 Project(B14041)
文摘Crystal structure and crystallinity of carbon nitride support, size and dispersity of active-metal nanoparticles(NPs), and surface engineering of composites have great roles in generation and separation of photogenerated charge carries and photocatalyzed organic reactions for the conversion of solar energy into chemical energy. Herein, we deposited well-dispersed Pd NPs with small size on crystallized carbon nitride(CN–C) to construct a Schottky-type Pd/CN–C hybrid for photocatalyzed Ullmann C–C homocoupling of aryl halides under visible light irradiation at room temperature. Compared to Pd NPs supported g-C_3N_4(Pd/g-C_3N_4), Pd/CN–C exhibits excellent visible light photocatalytic activity for Ullmann C–C coupling of aryl halides due to high crystallinity of CN–C support, high dispersion and smaller size of Pd NPs, and the interfacial heterojunction of Pd/CN–C. Upon visible light irradiation, more photogenerated electrons from CN–C flow across the Schottky junction to metallic Pd and trigger the Ullmann C–C coupling of aryl halides. The photogenerated holes on CN–C surface are captured by a protic solvent(such as EtOH). In the presence of base K_2CO_3, the solvent undergoes dissociation, dehydrogenation, and finally can be oxidized by captured photogenerated holes. Moreover, Pd/CN–C has general applicability for various substrates and shows excellent stability and reusability for more than nine cycles.
文摘The processing of an energy carrier such as microalgae oil into valuable fuels and chemicals is quite promising.Aqueous-phase processing is suitable for this purpose because the separation of intrinsic water from the algae cell is difficult.In this study,we synthesized ruthenium(Ru)nanoparticles supported on highly hydrophilic mesoporous carbon to catalyze the quantitative hydrodeoxygenation(HDO)of microalgae oil to alkanes in a one-pot process at a low temperature(140℃)in the aqueous phase.The mesoporous carbon was obtained by single-step calcination of starch and zinc chloride in nitrogen.The as-obtained carbon showed high surface areas and pore volumes,allowing high dispersion of Ru nanoparticles.The surface of the carbon material was rich in hydroxyl groups,as evidenced by X-ray photoelectron spectroscopy(XPS),infrared(IR)spectroscopy,and thermogravimetric analysis(TGA)measurements.As a result,the carbon material contacted preferably with the water phase versus the organic phase,improving the accessibility of substrates.On the other hand,the contact angle test results speculated the superior hydrophilic nature of mesoporous Ru/C(ZnCl2,starch)than commercial Ru/C.Both kinetics modeling and in situ IR monitoring in water revealed the superior performance of the hydrophilic mesoporous and hydrophilic Ru/C compared to a commercial Ru/C for the tandem hydrogenation of stearic acid and decarbonylation of stearyl alcohol.The herein designed hydrothermal carbon material was highly active,environmentally benign,sustainable,and recyclable material,and could be potentially used for other hydrogenation reactions in the aqueous phase.