Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and amel...
详细信息
Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.
Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution re...
详细信息
Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution reaction(HER)competition in this process prominently decreases C2H4 selectivity,thereby hindering its practical ***,a Cu-based composite catalyst,wherein porous carbon with nanoscale pores was used as a support,is constructed to gather the C_(2)H_(2) feedstocks for suppressing the undesirable *** a result,the as-prepared catalyst exhibited C_(2)H_(2) conversion of 27.1%and C_(2)H_(4) selectivity of 88.4%at a C2H4 partial current density of 0.25 A/cm^(2) under optimal−1.0 V versus reversible hydrogen electrode(RHE)under the simulated coal-derived C_(2)H_(2) atmosphere,significantly outperforming the single Cu NPs *** addition,a series of in situ and ex situ experimental results show that not only the porous nature of the carbon support but also the stabilized Cu^(0)–Cu^(+) dual active sites through the strong metal–support interactions enhance the adsorption capacity of C_(2)H_(2),leading to high C_(2)H_(2) partial pressure,restraining the HER and thus improving the C2H4 selectivity.
Understanding and manipulating synthetic progress for precisely controlling the components and defects of nanomaterials is an important and challenging task in materials synthesis and *** phosphides(MPs)have been expl...
详细信息
Understanding and manipulating synthetic progress for precisely controlling the components and defects of nanomaterials is an important and challenging task in materials synthesis and *** phosphides(MPs)have been explored as cheap advanced materials in various catalytic *** materials are usually synthesized through gas-solid phosphorization reaction in a trial-to-error manner,but their formation mechanism and the origin of controlled synthesis remain ***,we combine in situ thermogravimetrc analysis-mass spectrometry(TG-MS)and quasi-in situ X-ray powder diffraction(XRD)analysis to probe the transformation mechanism from metal oxides(MOs)to MPs during the phosphorization process mediated by ***,time,and the amount of hypophosphite are revealed as the driven forces while oxophilicity and crystallinity as the impeded forces,simultaneously control the component and defect level of a series of MP(M=Ni,Co,W,Mo,and Nb).The as-obtained WO2.9/WP is proved to be an efficient Z-scheme photocatalyst for oxidative coupling of methane with the total C2+production and C2H4 selectivity in C2+products reaching 10.75 pmolg-1 and 98.25%.Our work provides a fundamental understanding of the phosphorization treatment and thereby guides a viable synthetic route to the controlled synthesis of MOx-δ,MP,MOx-δ/MP,and MP/M heterostructured materials.
Electrocatalytic nitric oxide(NO)reduction is a promising strategy to produce *** a facile approach to synthesize efficient catalysts with enhanced NO electroreduction performance is highly ***,a series of Ru-doped Cu...
详细信息
Electrocatalytic nitric oxide(NO)reduction is a promising strategy to produce *** a facile approach to synthesize efficient catalysts with enhanced NO electroreduction performance is highly ***,a series of Ru-doped Cu materials are constructed through in situ electroreduction of corresponding metal *** optimized Ru_(0.05)Cu_(0.95)exhibits superior electrocatalytic performance for ammonia synthesis by using NO/Ar(1/4,n/n)as the feedstocks(Faradaic efficiency:64.9%,yield rate:17.68μmol cm^(-2)h^(-1)),obviously outperforming Cu counterpart(Faradaic efficiency:33.0%,yield rate:5.73μmol cm^(-2)h^(-1)).Electrochemical in situ Fourier transform infrared(FTIR)spectroscopy and online differential electrochemical mass spectrometry(DEMS)are adopted to detect intermediates and unveil the possible reaction *** downshift of the Cu d-band center induced by Ru doping facilitates the rate-limiting hydrogenation step and decreases the desorption energy of NH_(3),leading to high Faradaic efficiency and yield of ammonia.
Battery electrochemistry in an actual cell is a complicated behavior influenced by the current density,uniformity,and ion-diffusion distance,*** anisotropism of the lithiation/delithiation degree is usually inevitable...
详细信息
Battery electrochemistry in an actual cell is a complicated behavior influenced by the current density,uniformity,and ion-diffusion distance,*** anisotropism of the lithiation/delithiation degree is usually inevitable,and even worse,due to a trend of big-size cell design,typically such as 4680 and blade cells,which accelerated a battery failure during repeat lithiation and delithiation of *** by that,two big-size pouch cells with big sizes,herein,are selected to reveal the ion-diffusion dependency of the cathodes at different ***,we find that the LiCoO_(2) pouch cell exhibits ~5 A h loss after 120 charge-discharge cycles,but a 15 A h loss is verified in a LiNixMnyCO_(1-x)-yO_(2)(NCM) ***-based imaging analysis indicates that higher ion-diffusion rates in the LiCoO_(2)than that in the LiNixMnyCO_(1-x)-yO_(2)is the determined factor for the anisotropic cathode fading,which is responsible for a severe mechanical issue of particle damage,such as cracks and even pulverization,in the cathode ***,we verify the different locations at the near-tab and bottom of the electrode make it worse due to the ion-diffusion kinetics and temperature,inducing a spatially uneven electrochemistry in the big-size pouch *** findings give an in-depth insight into pouch cell failure and make a guideline for high-energy cell design and development.
According to the geological and mining conditions of deep high gas coal seam,this paper established the mechanical model of stope surrounding rock,and analyzed the stress distribution and deformation failure mechanism...
详细信息
According to the geological and mining conditions of deep high gas coal seam,this paper established the mechanical model of stope surrounding rock,and analyzed the stress distribution and deformation failure mechanism of working face and coal *** research determined the arrangement mode that adjacent working faces retain wide pillar,and the reasonable support method of roadway that the combined support of roof and grouting combined *** reasonable time of reinforced roadway was *** analyzing the mechanical model of the ways of roadway supporting,this research drew the conclusions as follows:the combined support of roof and working slope improved the support strength and range of surrounding rock,optimized the support by adjusting the angle of anchor,and reached the support requirements by using cement grouting in working slope and chemical grout in *** technology was applied in 15104 working face of Baoan Mine,and obtained good results.
As a vital nutrient closely related to the cance r-cells proliferation,phosphate anions have been paid great attention as a promising anticancer ***,the transport of phosphate anions depends on a protein transport sys...
详细信息
As a vital nutrient closely related to the cance r-cells proliferation,phosphate anions have been paid great attention as a promising anticancer ***,the transport of phosphate anions depends on a protein transport system which is regulated by ion homeostasis ***,we designed a reactive anionic nanocarrier based on black phosphorus nanosheets(BPs)and artesunate(ART),which could enter cells through endocytosis to generate phosphate anions,avoiding the regulation of cell *** ionic nanocarrier was coated by polydopamine to defend BPs and ART and functionalized by folate(FA)and hyaluronic acid(HA)for targeting *** the anchoring groups FA/HA targeted the carrier into cells,polydopamine coating decomposed to expose ART for further generating reactive oxygen species(ROS)in cancer cell microenvironment,providing oxidation ***,ROS generated by ART makes BPs decompose to phosphate anions with effectively speed,giving rise to the destruction of ion homeostasis to induce necro sis and inhibit the proliferation for cancer *** consequence,this research provides novel idea and direction for the ionic carriers and tumor therapeutics.
The effect of hydroxyl radical(·OH) on microalgae in ballast water is experimentally investigated. An ?OH plasma generator, which has a thin plate discharge Ag electrode covered by two α-Al2 O3 dielectric layers, is...
详细信息
The effect of hydroxyl radical(·OH) on microalgae in ballast water is experimentally investigated. An ?OH plasma generator, which has a thin plate discharge Ag electrode covered by two α-Al2 O3 dielectric layers, is built. The plasma generator is filled with O2 and gaseous H2 O and is powered by a homemade power supply. ?OH radicals are generated by a series of plasma reactions and then dissolved into ballast water to kill microalgae. The maximum density of the killed microalgae is about 11 000 cells per milliliter. At this density, the microalgae are not reactivated at the 48th hour and the 120th hour in the treated ballast waters, and the content of chlorophyll in these microalgae decreases by 100%. The water quality returns to a normal level after 120 hours without secondary pollution of aquatic organisms and environment. These results show that the requirements of the D-2 ballast water discharge standard defined by the International Maritime Organization(IMO) are satisfied with the proposed treatment, and that ·OH is an ideal substance for killing microalgae during ballast water replacement of ships.
暂无评论