摘要：The efficient and stable abatement of CO pollutant under ambient conditions is of great significance;however,it remains a formidable ***,we report the versatile application of wet oxidation over Fe(OH)x supported subnanometer Pt group metal(PGM)catalysts for the complete removal of CO under ambient temperature and humidity ***,the 1.8 wt%Rh/Fe(OH)x catalyst exhibited better durability during a^1400 min run for wet oxidation than for dry CO *** characterization results including HR-TEM,H2-TPR,and in-situ DRIFTS suggested that Fe(OH)x,with good reducibility,promoted by the subnanometer Rh clusters,provided sites for the adsorption and reaction of O2 and H2 O to form OH ***,these OH species reacted with the adsorbed CO on Rh sites with a considerably lower activation energy(9 kJ mol^-1)than that of dissociated 0 species(22 kJ mol^-1),thus rationalizing the outstanding performance of Rh/Fe(OH)x for wet *** experiments with other PGMs revealed a good generality for the application of wet oxidation in the efficient abatement of CO under humid conditions with Fe(OH)x as the support.

摘要：金属有机骨架(MOFs)衍生的Co基催化剂用于芳香硝基化合物选择加氢引起了广泛的关注,但催化剂合成过程中使用大量溶剂,且对催化剂中活性中心的认识存在争议.本文开发了一种固相合成策略,在不使用任何溶剂的情况下获得MOF前体材料,经发泡和热解处理获得Co@NC催化剂.研究发现,800℃热解所得的催化剂中Co纳米颗粒被氮掺杂石墨烯壳层包裹,在3-硝基苯乙烯的加氢过程中表现出~100%的转化率,3-乙烯基苯胺的选择性大于99%,同时,该催化剂具有良好的循环稳定性和底物普适性.表征和实验结果证明该催化剂中Co–N物种为活性中心,其含量可通过热解温度进行调变,且催化性能与Co–N物种的含量存在正相关关系.本工作为设计用于选择加氢反应的高效Co基催化剂提供了一种新的绿色合成策略.

摘要：Chemoselective hydrogenation of unsaturated aldehyde to unsaturated alcohol has attracted growing interests in recent years due to its widespread applications in fine ***,the hydrogenation of the C=O bond was thermodynamically and kinetically unfavorable over the hydrogenation of the C=C ***,to obtain the unsaturated alcohol from the unsaturated aldehyde is very difficult in most of the catalytic *** this work,ZnAl-hydrotalcite-supported cysteine-capped Au25 nanoclusters were used as the precatalysts for chemoselective hydrogenation of cinnamaldehyde to cinnamyl *** catalyst showed stable high selectivity(~95%)at prolonged reaction time and complete conversion of the *** to the results of the control experiments,the in-situ DRIFTS of the substrate under high pressure of hydrogen and the 27Al MAS-NMR spectroscopy,we proposed that the difference of the preferential adsorption of the C=O bond to that of the C=C bond was derived from the nature of the support of the gold catalysts.

摘要：The structure of Ni active sites supported on amorphous silica-alumina supports with different contents of Al_(2)O_(3)loadings in relation to their activities in ethylene oligomerization were *** kinds of Ni sites were detected by in situ FTIR-CO and H_(2)-TPR experiments,that are Ni^(2+)cations as grafted on weak acidic silanols and Ni^(2+)cations at ion-exchange *** ethylene oligomerization activities of these Ni/ASA catalysts were found an ascending tendency as the Al_(2)O_(3)loading decreased,which could be attributed to the enriched concentration of Ni^(2+)species on acidic silanols with a weaker interaction with the amorphous silica-alumina *** Ni^(2+)species were more easily to be evolved into Ni^(+)species,which has been identified to be the active sites of ethylene ***,it seems reasonable to conclude that Ni^(2+)species grafted on acidic silanols were the precursors of active sites.

摘要：Electrochemical CO2 reduction to chemicals or fuels presents one of the most promising strategies for managing the global carbon balance, which yet poses a significant challenge due to lack of efficient and durable electrocatalyst as well as the understanding of the CO2 reduction reaction(CO2RR) *** from the large surface area, high electrical conductivity, and tunable structure, carbon-based metal-free materials(CMs) have been extensively studied as cost-effective electrocatalysts for *** development of CMs with low cost, high activity and durability for CO2RR has been considered as one of the most active and competitive directions in electrochemistry and material *** this review article,some up-to-date strategies in improving the CO2RR performance on CMs are ***, the approaches to optimize the adsorption of CO2RR intermediates, such as tuning the physical and electronic structure are introduced, which can enhance the electrocatalytic activity of CMs ***, some design strategies are proposed to prepare CMs with high activity and selectivity for CO2RR.

摘要：Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and ***,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers,resulting in slow reaction kinetics and limited CO_(2)***,we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS *** novel material achieved an unprecedented CO production rate of 381 mL g^(-1)min^(-1)with 99%CO_(2)conversion at 850℃,outperforming state-of-the-art *** situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO_(2)*** oxidation of the FeNi alloy at the interface(as opposed to forming an FeO_(x)passivation shell encapsulating bare metallic iron)and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO_(2)to *** regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas(H_(2)/CO=2,syngas yield>96%).Overall,the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production,with a theoretical solar-to-fuel efficiency of up to 58%,in the absence of any heat integration.

摘要：The catalytic hydrogenation of halonitroarenes to haloanilines is a green and sustainable process for the production of key nitrogen-containing intermediates in fine chemical *** hydrogenation poses a significant challenge,which requires the rational design of the catalysts with proper hydrogenation ability for nitro group and simultaneously preventing dehalogenation of halogen ***,a highly effective Rh@Al_(2)O_(3)@C single-atom catalyst(SAC)was developed for the hydrogenation of m-chloronitrobenzene(m-CNB)to m-chloroaniline(m-CAN),through an in-situ grafting of metal during the assembly of MIL-53(Al),followed by confined *** characterizations reveal an exquisite structure of the Rh@Al_(2)O_(3)@C,containing atomically dispersed Rh sites onto Al_(2)O_(3) confined by the amorphous *** five-coordinated aluminum(Al^(Ⅴ))species are essential for achieving the atomic dispersion of Rh atoms,providing the unsaturated coordinative sites for *** to the benchmark Rh/γ-Al_(2)O_(3) and Rh/C nanocatalysts,the Rh@Al_(2)O_(3)@C SAC affords an excellent turnover frequency of 2317 molm-CNB·molRh^(–1)·h^(–1),the highest value to date in heterogeneous catalyst systems for the hydrogenation of m-CNB at 313 K and 20 bar H2,together with a sustained selectivity to m-CAN(~98%)during five consecutive *** superior catalytic performance of the Rh@Al_(2)O_(3)@C is attributed to a proper modulation of electronic structure of hydrogenation metal by forming SAC,together with an enhanced accessibility of acid function sites.