摘要：X-ray diffraction enhanced imaging （DEI） has extremely high sensitivity for weakly absorbing low- Z samples in medical and biological fields. In this paper, we propose an Algebra Reconstruction Technique （ART） iterative reconstruction algorithm for computed tomography of diffraction enhanced imaging （DEI-CT）. An Ordered Subsets （OS） technique is used to accelerate the ART reconstruction. Few-view reconstruction is also studied, and a partial differential equation （PDE） type filter which has the ability of edge-preserving and denoising is used to improve the image quality and eliminate the artifacts. The proposed algorithm is validated with both the numerical simulations and the experiment at the beijing synchrotron radiation facility （BSRF）.

摘要：Hierarchical Pt-alloys enriched with active sites are highly desirable for efficient catalysis,but their syntheses generally need time-consuming and elaborate annealing treatment at high *** herein report a surface active-site engineering strategy for constructing the hierarchical PtNi nanocatalysts with an atomic Pt-skin layer(PtNi@Pt-SL)towards efficient triiodide reduction reaction(TRR)via an acid-dealloying *** facile acid-dealloying process promotes the formation of surface Pt active sites on the hierarchical Pt-alloys,and thus results in good catalytic performance towards *** calculation reveals that the enhanced catalytic property stems from the moderate energy barriers for iodide atoms on the surface Pt *** surface active-site engineering strategy paves a new way for the design of active and durable electrocatalysts.

摘要：K-ion batteries(KIBs)hold great promise for large-scale energy ***,the absence of suitable cathode materials limits their practical ***,rationally designing advanced cathode materials for KIBs remains an open *** this work,based on density functional theory calculations,we find that the bond stability of Fe–O is higher than that of Co–O in layered transitional metal(TM)***,the K-ion migration in the Fe-based layered TM oxide has a significantly lower activation energy barrier than that in the Co-based *** on this theoretical prediction,we successfully synthesized a low-cost K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2)cathode,which shows excellent structural stability and superior K-storage properties,including durable cycle life and high-rate ***,the designed K_(0.45)Ni_(0.1)Fe_(0.1)Mn_(0.8)O_(2)cathode possesses a great full-cell performance with a discharge capacity of~75 mA h g^(-1) and capacity retention of~80%after 100 *** results show that Fe has better structural stability and K-ion diffusion than high-cost Co in layered oxide cathodes,and this finding provides new insights into the design of low-cost and high-performance KIB layered *** work highlights the feasibility of a theory-guided experiment in screening promising battery materials.

摘要：The rational design of efficient single-atomic(SA)catalysts is essential and highly desirable but impeded by the lack of sufficient acknowledge between structure and *** this end,it is critical to clarify the effect of the coordination structure of active metal centers on the catalytic activities for the design of such ***,we report that different coordination structures of SA Pt catalysts can dramatically influence their activities for anti-Markovnikov hydroboration of *** with the other two coordination structures(Pt-N4 and Pt-O2),the SA Pt species coordinated with three O atoms(Pt-O3)display the highest turnover number value of 3288 for the hydroboration reaction to access the important alkylboronic *** functional theory calculations reveal that a superior catalytic activity can be expected for alkene hydroboration over the three O coordinated Pt species due to the lowest reaction energy(ΔG)limiting step from the reaction phase diagram.

摘要：Photoelectrochemical(PEC)water splitting for solar energy conversion into chemical fuels has attracted intense research *** semiconductor hematite(α-Fe_(2)O_(3)),with its earth abundance,chemical stability,and efficient light harvesting,stands out as a promising photoanode ***,its electron affinity is too deep for overall water splitting,requiring additional *** engineering has been used to reduce the onset potential of hematite *** we focus instead on energy band engineering hematite by shrinking the crystal lattice,and the water-splitting onset potential can be decreased from 1.14 to 0.61 V *** reversible hydrogen *** is the lowest record reported for a pristine hematite photoanode without surface modification.X-ray absorption spectroscopy and magnetic properties suggest the redistribution of 3d electrons in the as-synthesized grey hematite *** function theory studies herein show that the smaller-lattice-constant hematite benefits from raised energy bands,which accounts for the reduced onset potential.

摘要：通过电催化氧化葡萄糖等可再生生物质生产高附加值化学品为实现碳中和目标提供了一条有效途径.目前用于电催化生物质氧化反应的电催化剂主要分为贵金属基催化剂和非贵金属基催化剂.对于贵金属基电催化剂,文献报道了铂基催化剂的氧化态随电势变化,进而调控电催化葡萄糖氧化的活性和选择性.对于非贵金属基催化剂,钴基和镍基氧化物和氢氧化物被广泛应用于电催化生物质氧化反应,但铜基催化剂直到最近才引起关注.最近,金属铜、氧化亚铜和氢氧化铜在内的铜基材料被证实是一类有应用前景的电催化生物质氧化催化剂,但在电化学条件下的真实活性位结构仍难以鉴定.本文针对电催化葡萄糖等生物质平台分子的氧化反应,证明了氧化铜的催化活性相随电压升高从氢氧化铜演变为羟基氧化铜,阐明了结构和反应活性及选择性的构效关系,该工作加深了对铜基催化剂活性位动态重构的理解,有助于电催化生物质转化的催化剂理性设计,促进可再生资源利用和碳中和目标的实现.

摘要：Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles （NPs） in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered the development of efficient catalysts for CO2 electroreduction. Herein, we report the systematic engineering of active phases of Pd NPs, which are exploited to select reaction pathways for CO2 electroreduction. In situ X-ray absorption spectroscopy, in situ attenuated total reflection-infrared spectroscopy, and density functional theory calculations suggest that the formation of a hydrogen-adsorbed Pd surface on a mixture of the α- and β-phases of a palladium-hydride core （α＋β PdHx@PdHx） above -0.2 V （vs. a reversible hydrogen electrode） facilitates formate production via the HCOO intermediate, whereas the formation of a metallic Pd surface on the β-phase Pd hydride core （β PdHx@Pd） below -0.5 V promotes CO production via the COOH＂ intermediate. The main product, which is either formate or CO, can be selectively produced with high Faradaic efficiencies （〉90%） and mass activities in the potential window of 0.05 to -0.9 V with scalable application demonstration.

摘要：The anionic redox chemistry(O^2-→O^-)in P2-type sodium-ion battery cathodes has attracted much ***,determining how to tune the anionic redox reaction is still a major ***,we tune the activity and reversibility of both the anionic and cationic redox reactions of Na0.67Mn0.5Fe0.5O2 though an integrated strategy that combines the advantages of Li2SiO3 coating,Li doping and Si doping,and the initial capacity,rate performance and cycling stability are significantly *** in-depth modulation mechanism is revealed by means of neutron diffraction,X-ray absorption spectroscopy,in situ X-ray diffraction,electron paramagnetic resonance spectroscopy,first-principles calculations and so *** Li2SiO3 coating alleviates the side reactions and enhances the cycling ***^4+doping lowers the Na^+diffusion barrier due to the expanded interlayer ***,Si^4+doping improves the structural stability,oxygen redox activity and ***^+doping in Na sites further increases the structure *** electron density maps confirm the greater activity of Na and O in the modified *** density maps and bond-valence energy landscapes identify the Na^+migration pathway from Nae site to Naf site(the positions of the Na ions in the crystal structure).The proposed insights into the modulation mechanism of the anionic and cationic redox chemistry are also instructive for designing other oxide-based cathode materials.

摘要：Herein,we report the excellent De-NO_(x)performance of La0.7Sr0.3MnO3(LSM)perovskite-supported Pd catalysts(Pd-LSM)in alternating lean-burn/fuel-rich atmospheres using C3H6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction(MSI)*** NO_(x)reduction conversion of the Pd-LSM catalyst increased significantly from 56.1%to 90.1%and the production of N2O was *** results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd2+into Pd0 during the *** generated Pd0 species could readily activate the C3H6 reductant and achieve an eight-fold higher turnover frequency than Pd2+for the reduction of NO_(x).Moreover,excessive MSIs inhibited the in situ generation of Pd0,and thereby,lowered the De-NO_(x)activity of the catalyst even at high Pd *** addition,the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al_(2)O_(3)-supported *** study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.

摘要：Two-dimensional layered double hydroxides(LDHs)have been identified as promising electrocatalysts for the oxygen evolution reaction(OER);however,the simple and effective synthesis of high-quality LDHs remains extremely challenging and the active sites have not been ***,we report a facile solution-reaction method for preparing an ultrathin(thickness<2 nm)nonprecious CoFe-based ***_(1)Fe_(0.2) LDH delivers a current density of 10 mA cm^(-2) and a high turnover frequency of 0.082 s^(-1) per total 3d metal atoms at a low overpotential of 256 *** mass activity is 277.9 A g^(-1) at an overpotential of 300 mV for the *** studies reveal the Co site as the main active center for the *** doped Fe lowers the reaction barrier by accelerating the charge-transfer *** calculations reveal that the surface Co sites adjacent to Fe atoms are the active centers for the OER and the subsurface Fe dopants excessively weaken the OH^(*)adsorption,thus increasing the energy barrier of the rate-determining *** study can guide the rational design of high-performance CoFe-based LDHs for water splitting.