The direct carbonylation of methanol, without any halide in the feed as apromoter, is presented. A series of Mo catalysts supported on activated carbon, γ-Al_2O_3 and SiO_2were prepared. The results show that the sup...The direct carbonylation of methanol, without any halide in the feed as apromoter, is presented. A series of Mo catalysts supported on activated carbon, γ-Al_2O_3 and SiO_2were prepared. The results show that the support greatly affects the Mo catalyst in the directvapor-phase carbonylation of methanol, and activated carbon is the best supports of the investigatedsupports. In addition, the relationships between adsorptions of NH_3 and CO and carbonylation ofmethanol were investigated. A novel sulfided Mo/C catalyst had high activity and selectivity for thevapor phase carbonylation of methanol to methyl acetate without the addition of a CH_3I promoter tothe feed. The reaction conditions were optimized at a reaction temperature of 573 K, a methanolconcentration of 23 mol% and a carbon monoxide space velocity of 3,000 L/(kg·h). Under theseoptimal conditions a methanol conversion of 50%, carbonylation selectivity of 80 rnol%, andspace-time yield of 8.0 mol/(kg·h) were obtained. The active phase of this novel sulfided Mo/Ccatalyst is the non-crystalline phase, and the active component is present as MoS_(2.5) on thesurface of the activated carbon.展开更多
Six Ni-Mo catalysts with different metal contents were prepared and characterized by N2 adsorption and X-ray diffi＇actometry. The active phase microstructure of these catalysts was examined by the Raman spectroscopy,...Six Ni-Mo catalysts with different metal contents were prepared and characterized by N2 adsorption and X-ray diffi＇actometry. The active phase microstructure of these catalysts was examined by the Raman spectroscopy, temperature- programmed reduction （TPR）, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. Hydrodesulfurization （HDS） activity of catalyst samples were analyzed in a flow fixed-bed microreactor. The sulfidation degree of Mo and the length of the MoS2 slab slightly increased with the amount of metal loaded following sulfidation. This small change is attributed to polymolybdate species observed in all the oxidized catalysts. Weak metal-support interactions, as determined by the TPR technique, increased the NiSx sulfidation phase and MoS2 slab stacking. The HDS activity of the catalyst samples increased with the number of active sites. For high metal loading catalysts, their HDS activity was nearly identical because the sulfur atoms cannot easily approach active sites. This change is caused by the large number of stacked layers in the MoS2 slabs as well as the decrease in the specific surface area and pore volume of the catalyst samples with an increasing metal loading.展开更多
Co-Mo/MgO-Al2O3 catalyst was presulfided with ammonium sulfide in aqueous solution and activated with synthesis gas for water gas shift reaction. The assay results indicate that the presulfided Co-Mo/MgO-Al2O3 catalys...Co-Mo/MgO-Al2O3 catalyst was presulfided with ammonium sulfide in aqueous solution and activated with synthesis gas for water gas shift reaction. The assay results indicate that the presulfided Co-Mo/MgO-Al2O3 catalyst exhibits an excellent catalytic activity and stability. XRD and EPR characterization results show that the O-S exchange might occur during the impregnation, leading to the formation of （NH4）2MoS4 （or （NH4）zMoxSy） precursor, which was then thermally decomposed and reduced to MoS2. The higher catalytic performance is attributed to an optimization formation of active Co-Mo sulfides, consisting of well dispersed MoS2 and Co-Mo-S phase due to the redispersion of Co sulfide particles over the edges of newly formed MoS2 crystallites.展开更多
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an...The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.展开更多
Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature&l...This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.展开更多
Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesi...Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesized via a facile approach involving the solvothermal method and subsequent sulfuration treatment.The resultant CuS/Cu_(9)S_(5) exhibited superb microwave absorbing capacity with a minimum reflection loss(RLmin)of-59.38 dB at 2.7 mm.The maximum effective absorption bandwidth(EABmax)was 7.44 GHz(10.56-18 GHz)when the thickness was reduced to 2.3 mm.The outstanding microwave absorbing ability of CuS/Cu_(9)S_(5) composites is mainly related to its unique hexapod shape and the formation of heterogeneous interfaces.The unique hexapod shape significantly promotes the multi-reflection of the incident electromagnetic wave(EMW)increasing the attenuation path of EMWs in the material.Hetero-geneous interfaces between CuS/Cu_(9)S_(5) enable powerful interface polarization,contributing to the atten-uation of EMWs propagating in the medium.In addition,the EMW absorption performance of CuS/Cu_(9)S_(5) composites is also inseparable from the conduction loss.This study provides a strong reference for the research of EMW absorbent materials based on transition metal sulfides.展开更多
Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poo...Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.展开更多
Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance...Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.展开更多
Transition metal sulfides have great potential as anode mterials for sodium-ion batteries(SIBs)due to their high theoretical specific capacities.However,the inferior intrinsic conductivity and large volume variation d...Transition metal sulfides have great potential as anode mterials for sodium-ion batteries(SIBs)due to their high theoretical specific capacities.However,the inferior intrinsic conductivity and large volume variation during sodiation-desodiation processes seriously affect its high-rate and long-cyde performance,unbeneficial for the application as fast-charging and long-cycling SIBs anode.Herein,the three-dimensional porous Cu_(1.81)S/nitrogen-doped carbon frameworks(Cu_(1.81)S/NC)are synthesized by the simple and facile sol-gel and annealing processes,which can accommodate the volumetric expansion of Cu_(1.81)S nanoparticles and accelerate the transmission of ions and electrons during Na^(+)insertion/extraction processes,exhibiting the excellent rate capability(250.6 mA·g^(-1)at 20.0 A·g^(-1))and outstanding cycling stability(70% capacity retention for 6000 cycles at 10.0 A·g^(-1))for SIBs.Moreover,the Na-ion full cells coupled with Na_(3)V_(2)(PO_(4))_(3)/C cathode also demonstrate the satisfactory reversible specific capacity of 330.5 mAh·g^(-1)at 5.0 A·g^(-1)and long-cycle performance with the 86.9% capacity retention at 2.0 A·g^(-1)after 750 cycles.This work proposes a promising way for the conversionbased metal sulfides for the applications as fast-charging sodium-ion battery anode.展开更多
The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge...The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.展开更多
Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate per...Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate performance,arising from volume expansion and structural degradation,remain sig-nificant challenges.We report a novel FeS_(2)/CoS_(2) heterostruc-ture embedded in a 3D carbon aerogel matrix(FeS_(2)/CoS_(2)@C)synthesized by a cross-linking and vulcanization process.The resulting core-shell structure,with bimetallic FeS_(2)/CoS_(2) nano-particles encapsulated in a conductive carbon shell,effectively reduces the adverse effects of volume changes during sodiation/desodiation cycles.The 3D porous carbon network increases both ion and electron diffusion,while preventing agglomeration of the active material and maintaining interface integrity.The FeS_(2)/CoS_(2)@C composite has an outstanding electrochemical performance,including a high specific capacity of 725 mAh g^(-1)at 0.5 A g^(-1)and an exceptional rate capability of 572 mAh g^(-1)at 10 A g^(-1).It also has remarkable cycling stability with no signific-ant capacity decay over 1000 cycles at 5 A g^(-1).展开更多
CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesi...CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesis process.Results show that CuS-C50 has the complete nanoflower structure.In aluminum chloride-pentamethylcydopentodiene/tetrahydrofuran(APC/THF)electrolyte,the CuS-C50 exhibits a high specific capacity of 331.19 mAh/g when the current density is 50 mA/g and still keeps a specific capacity of 136.92 mAh/g over 50 cycles when the current density is 200 mA/g.Results of morphology characterizations indicate that the complete nanoflower structure can provide more active sites and reduce the barriers for Mg^(2+)movement,eventually improving the charge and discharge performance of the CuS cathode materials for magnesium ion batteries.展开更多
Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an excep...Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an exceptionalspecific capacitance of 190.8 mAh·g^(-1)at 1 A·g^(-1),greatly higher than the corresponding monometallic sulfides MnS(31.7 mAh·g^(-1))and Co_(3)S_(4)(86.7 mAh·g^(-1)).Impressively,the as-assembled MnCo_(2)S_(4)||porous carbon(PC)hybridsupercapacitor(HSC),showed an outstanding energy density of 76.88 Wh·kg^(-1)at a power density of 374.5 W·kg^(-1),remarkable cyclic performance with a capacity retention of 86.8% after 10000 charge-discharge cycles at 5 A·g^(-1),and excellent Coulombic efficiency of 99.7%.展开更多
The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nit...The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.展开更多
Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite end...Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite endows it with abundant catalytically active sites,thereby accelerating the reduction of I_(3)^(-).More importantly,the dye-sensitized solar cells(DSSCs)prepared by scraping it on flexible titanium mesh with low resistance had low series resistance(Rs).Electrochemical characterizations revealed that the DSSCs employing the FMS/CC counter electrode achieved a power conversion efficiency(PCE)of ca.9.51%(surpassing the ca.8.15%efficiency of the Pt counter electrode),open-circuit voltage(Voc)of ca.0.79 V,short-circuit current density(Jsc)of ca.18.31 mA·cm^(-2),and fill factor(FF)of ca.0.65.Moreover,after 100 times of cyclic voltammetry(CV)test,the CV curve remained unchanged,indicating the excellent stability of FMS/CC in the electrolyte containing I_(3)^(-)/I^(-).展开更多
Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether ...Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.展开更多
Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle...Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle size and settling performance remain unclear.In this study,the growth behavior of CuS particles generated by two sulfide precipitation methods,gas-liquid and liquid-liquid sulfidation,was investigated.The effects of acidity,sulfur-to-copper molar ratio,and temperature on particle size were analyzed.The results showed that increasing the temperature had an adverse effect on CuS particle growth.Additionally,we found that acidity and sulfur-to-copper molar ratio had a more significant impact on particle growth in the liquid-liquid sulfidation system than in the gas-liquid sulfidation system.Based on supersaturation calculations and XPS analysis,it is found that particle growth in gas-liquid sulfidation systems is mainly influenced by supersaturation,while particle growth in liquid-liquid sulfidation systems is mainly affected by surface charge.This study provides valuable insights into the factors that influence particle growth in sulfide precipitation and can inform the development of strategies to improve the effective precipitation of sulfide nanoparticles in acidic wastewater.展开更多
The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transitio...The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.展开更多
High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S...High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S under abundant biomass has been reported in these presumed steam sterilized reservoirs ever before.In this study,we propose a new mechanism,biomass thermal decomposition for sulfur compounds(BTDS),to interpret the increasing of sH_(2)S.Sulfur of cells' dry weight took 0.20%-1.92% of the active strains isolated from the in-situ thermal recovery reservoirs of Liaohe Oilfield.When microbial organic sulfur compounds(MOSC) in biomass were exposed to injected steam,it resulted in the BTDS process.The isolated Bacillus subtilis D3(G+) and Pseudomonas aeruginosa XJ14(G-) were chosen to simulate this process.About 36% of sulfur in MOSC emitted as H_(2)S in steam chamber by BTDS.The δ^(34)S of H_(2)S from produced gas ranged from 8.7‰ to 17.0‰,close to the δ^(34)S of H_(2)S 11.2‰ from BTDS simulation experiment.It provides new insight into the contribution and sulfur cycle made by subterranean microorganisms on H_(2)S formation.展开更多
基金This work was supported by the National Nature Science Foundation of China (No.29903003).
文摘The direct carbonylation of methanol, without any halide in the feed as apromoter, is presented. A series of Mo catalysts supported on activated carbon, γ-Al_2O_3 and SiO_2were prepared. The results show that the support greatly affects the Mo catalyst in the directvapor-phase carbonylation of methanol, and activated carbon is the best supports of the investigatedsupports. In addition, the relationships between adsorptions of NH_3 and CO and carbonylation ofmethanol were investigated. A novel sulfided Mo/C catalyst had high activity and selectivity for thevapor phase carbonylation of methanol to methyl acetate without the addition of a CH_3I promoter tothe feed. The reaction conditions were optimized at a reaction temperature of 573 K, a methanolconcentration of 23 mol% and a carbon monoxide space velocity of 3,000 L/(kg·h). Under theseoptimal conditions a methanol conversion of 50%, carbonylation selectivity of 80 rnol%, andspace-time yield of 8.0 mol/(kg·h) were obtained. The active phase of this novel sulfided Mo/Ccatalyst is the non-crystalline phase, and the active component is present as MoS_(2.5) on thesurface of the activated carbon.
基金SINOPEC for its financial support(No.108012/No.108041)
文摘Six Ni-Mo catalysts with different metal contents were prepared and characterized by N2 adsorption and X-ray diffi＇actometry. The active phase microstructure of these catalysts was examined by the Raman spectroscopy, temperature- programmed reduction （TPR）, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. Hydrodesulfurization （HDS） activity of catalyst samples were analyzed in a flow fixed-bed microreactor. The sulfidation degree of Mo and the length of the MoS2 slab slightly increased with the amount of metal loaded following sulfidation. This small change is attributed to polymolybdate species observed in all the oxidized catalysts. Weak metal-support interactions, as determined by the TPR technique, increased the NiSx sulfidation phase and MoS2 slab stacking. The HDS activity of the catalyst samples increased with the number of active sites. For high metal loading catalysts, their HDS activity was nearly identical because the sulfur atoms cannot easily approach active sites. This change is caused by the large number of stacked layers in the MoS2 slabs as well as the decrease in the specific surface area and pore volume of the catalyst samples with an increasing metal loading.
文摘Co-Mo/MgO-Al2O3 catalyst was presulfided with ammonium sulfide in aqueous solution and activated with synthesis gas for water gas shift reaction. The assay results indicate that the presulfided Co-Mo/MgO-Al2O3 catalyst exhibits an excellent catalytic activity and stability. XRD and EPR characterization results show that the O-S exchange might occur during the impregnation, leading to the formation of （NH4）2MoS4 （or （NH4）zMoxSy） precursor, which was then thermally decomposed and reduced to MoS2. The higher catalytic performance is attributed to an optimization formation of active Co-Mo sulfides, consisting of well dispersed MoS2 and Co-Mo-S phase due to the redispersion of Co sulfide particles over the edges of newly formed MoS2 crystallites.
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
文摘This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.
基金supported by the National Natural Science Foundation of China(Nos.52377026 and 52301192)the Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202103057)+3 种基金the Postdoctoral Fellow-ship Program of CPSF under Grant Number(No.GZB20240327)the Shandong Postdoctoral Science Foundation(No.SDCX-ZG-202400275)the Qingdao Postdoctoral Application Research Project(No.QDBSH20240102023)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Structural-Functional Polymer Composites).
文摘Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesized via a facile approach involving the solvothermal method and subsequent sulfuration treatment.The resultant CuS/Cu_(9)S_(5) exhibited superb microwave absorbing capacity with a minimum reflection loss(RLmin)of-59.38 dB at 2.7 mm.The maximum effective absorption bandwidth(EABmax)was 7.44 GHz(10.56-18 GHz)when the thickness was reduced to 2.3 mm.The outstanding microwave absorbing ability of CuS/Cu_(9)S_(5) composites is mainly related to its unique hexapod shape and the formation of heterogeneous interfaces.The unique hexapod shape significantly promotes the multi-reflection of the incident electromagnetic wave(EMW)increasing the attenuation path of EMWs in the material.Hetero-geneous interfaces between CuS/Cu_(9)S_(5) enable powerful interface polarization,contributing to the atten-uation of EMWs propagating in the medium.In addition,the EMW absorption performance of CuS/Cu_(9)S_(5) composites is also inseparable from the conduction loss.This study provides a strong reference for the research of EMW absorbent materials based on transition metal sulfides.
基金supported by the Science and Technology Department of Guangxi Zhuang Autonomous[grant numbers 2025GXNSFFA069003]the National Natural Science Foundation of China[grant numbers 22379030]+1 种基金Bagui Young Scholars Program of Guangxi Zhuang Autonomous Regionthe high-performance computing platform of Guangxi University.
文摘Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.
基金supported by the National Natural Science Foundation of China(Nos.22171180,22461142137,and 22478242)the Shanghai Municipal Science and Technology Major Project,China.
文摘Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.
基金financially supported by the National Natural Science Foundation of China(Nos.U1904173 and 52272219)the Key Research Projects of Henan Provincial Department of Education(No.19A150043)+2 种基金the Natural Science Foundation of Henan Province(Nos.202300410330 and 222300420276)the Nanhu Scholars Program for Young Scholars of Xinyang Normal Universitythe Xinyang Normal University Analysis&Testing Center。
文摘Transition metal sulfides have great potential as anode mterials for sodium-ion batteries(SIBs)due to their high theoretical specific capacities.However,the inferior intrinsic conductivity and large volume variation during sodiation-desodiation processes seriously affect its high-rate and long-cyde performance,unbeneficial for the application as fast-charging and long-cycling SIBs anode.Herein,the three-dimensional porous Cu_(1.81)S/nitrogen-doped carbon frameworks(Cu_(1.81)S/NC)are synthesized by the simple and facile sol-gel and annealing processes,which can accommodate the volumetric expansion of Cu_(1.81)S nanoparticles and accelerate the transmission of ions and electrons during Na^(+)insertion/extraction processes,exhibiting the excellent rate capability(250.6 mA·g^(-1)at 20.0 A·g^(-1))and outstanding cycling stability(70% capacity retention for 6000 cycles at 10.0 A·g^(-1))for SIBs.Moreover,the Na-ion full cells coupled with Na_(3)V_(2)(PO_(4))_(3)/C cathode also demonstrate the satisfactory reversible specific capacity of 330.5 mAh·g^(-1)at 5.0 A·g^(-1)and long-cycle performance with the 86.9% capacity retention at 2.0 A·g^(-1)after 750 cycles.This work proposes a promising way for the conversionbased metal sulfides for the applications as fast-charging sodium-ion battery anode.
文摘The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.
文摘Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate performance,arising from volume expansion and structural degradation,remain sig-nificant challenges.We report a novel FeS_(2)/CoS_(2) heterostruc-ture embedded in a 3D carbon aerogel matrix(FeS_(2)/CoS_(2)@C)synthesized by a cross-linking and vulcanization process.The resulting core-shell structure,with bimetallic FeS_(2)/CoS_(2) nano-particles encapsulated in a conductive carbon shell,effectively reduces the adverse effects of volume changes during sodiation/desodiation cycles.The 3D porous carbon network increases both ion and electron diffusion,while preventing agglomeration of the active material and maintaining interface integrity.The FeS_(2)/CoS_(2)@C composite has an outstanding electrochemical performance,including a high specific capacity of 725 mAh g^(-1)at 0.5 A g^(-1)and an exceptional rate capability of 572 mAh g^(-1)at 10 A g^(-1).It also has remarkable cycling stability with no signific-ant capacity decay over 1000 cycles at 5 A g^(-1).
基金National Natural Science Foundation of China(52171101)Fundamental Research Funds for the Central Universities(2024IAIS-QN009)National Key R&D Program of China(2021YFB3701100)。
文摘CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesis process.Results show that CuS-C50 has the complete nanoflower structure.In aluminum chloride-pentamethylcydopentodiene/tetrahydrofuran(APC/THF)electrolyte,the CuS-C50 exhibits a high specific capacity of 331.19 mAh/g when the current density is 50 mA/g and still keeps a specific capacity of 136.92 mAh/g over 50 cycles when the current density is 200 mA/g.Results of morphology characterizations indicate that the complete nanoflower structure can provide more active sites and reduce the barriers for Mg^(2+)movement,eventually improving the charge and discharge performance of the CuS cathode materials for magnesium ion batteries.
文摘Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an exceptionalspecific capacitance of 190.8 mAh·g^(-1)at 1 A·g^(-1),greatly higher than the corresponding monometallic sulfides MnS(31.7 mAh·g^(-1))and Co_(3)S_(4)(86.7 mAh·g^(-1)).Impressively,the as-assembled MnCo_(2)S_(4)||porous carbon(PC)hybridsupercapacitor(HSC),showed an outstanding energy density of 76.88 Wh·kg^(-1)at a power density of 374.5 W·kg^(-1),remarkable cyclic performance with a capacity retention of 86.8% after 10000 charge-discharge cycles at 5 A·g^(-1),and excellent Coulombic efficiency of 99.7%.
基金partially supported by National Natural Science Foundation of China(52172250)Institute of Process Engineering(IPE)Project for Frontier Basic Research(QYJC-2023-06)。
文摘The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.
文摘Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite endows it with abundant catalytically active sites,thereby accelerating the reduction of I_(3)^(-).More importantly,the dye-sensitized solar cells(DSSCs)prepared by scraping it on flexible titanium mesh with low resistance had low series resistance(Rs).Electrochemical characterizations revealed that the DSSCs employing the FMS/CC counter electrode achieved a power conversion efficiency(PCE)of ca.9.51%(surpassing the ca.8.15%efficiency of the Pt counter electrode),open-circuit voltage(Voc)of ca.0.79 V,short-circuit current density(Jsc)of ca.18.31 mA·cm^(-2),and fill factor(FF)of ca.0.65.Moreover,after 100 times of cyclic voltammetry(CV)test,the CV curve remained unchanged,indicating the excellent stability of FMS/CC in the electrolyte containing I_(3)^(-)/I^(-).
基金financially supported by the Natural Science Foundation of Jiangsu Province(Grant No.BK20241181)the State Key Laboratory of AnalyticalChemistry for Life Science,School of Chemistry and Chemical Engineering,Nanjing University(Grant No.SKLACLS2419)。
文摘Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.
基金supported by the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.52121004)the National Natural Science Foundation of China(No.52274414).
文摘Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle size and settling performance remain unclear.In this study,the growth behavior of CuS particles generated by two sulfide precipitation methods,gas-liquid and liquid-liquid sulfidation,was investigated.The effects of acidity,sulfur-to-copper molar ratio,and temperature on particle size were analyzed.The results showed that increasing the temperature had an adverse effect on CuS particle growth.Additionally,we found that acidity and sulfur-to-copper molar ratio had a more significant impact on particle growth in the liquid-liquid sulfidation system than in the gas-liquid sulfidation system.Based on supersaturation calculations and XPS analysis,it is found that particle growth in gas-liquid sulfidation systems is mainly influenced by supersaturation,while particle growth in liquid-liquid sulfidation systems is mainly affected by surface charge.This study provides valuable insights into the factors that influence particle growth in sulfide precipitation and can inform the development of strategies to improve the effective precipitation of sulfide nanoparticles in acidic wastewater.
基金supported by the Science and Technology Project of Southwest Petroleum University(No.2021JBGS03)the Local Science and Technology Development Fund Projects Guided by the Central Government of China(No.2021ZYD0060)+2 种基金the National Natural Science Foundation of China(Nos.22209143 and 52371241)Guangdong High-level Innovation Institute Project(Nos.2021B0909050001 and 2021CX02L365)Guangdong Basic and Applied Basic Research Foundation(No.2023B1515120095).
文摘The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.
文摘High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S under abundant biomass has been reported in these presumed steam sterilized reservoirs ever before.In this study,we propose a new mechanism,biomass thermal decomposition for sulfur compounds(BTDS),to interpret the increasing of sH_(2)S.Sulfur of cells' dry weight took 0.20%-1.92% of the active strains isolated from the in-situ thermal recovery reservoirs of Liaohe Oilfield.When microbial organic sulfur compounds(MOSC) in biomass were exposed to injected steam,it resulted in the BTDS process.The isolated Bacillus subtilis D3(G+) and Pseudomonas aeruginosa XJ14(G-) were chosen to simulate this process.About 36% of sulfur in MOSC emitted as H_(2)S in steam chamber by BTDS.The δ^(34)S of H_(2)S from produced gas ranged from 8.7‰ to 17.0‰,close to the δ^(34)S of H_(2)S 11.2‰ from BTDS simulation experiment.It provides new insight into the contribution and sulfur cycle made by subterranean microorganisms on H_(2)S formation.
