Diatomic-site catalysts (DACs) garner tremendous attention for selective CO photoreduction, especially in the thermodynamical and kinetical mechanism of CO to C products. Herein, we first engineer a novel Zn-porphyrin/RuCu-pincer complex DAC (ZnPor-RuCuDAC). The heteronuclear ZnPor-RuCuDAC exhibits the best acetate selectivity (95.
View Article and Find Full Text PDFInvited for the cover of this issue are Xiao-Yu Yang and co-workers at Wuhan University of Technology, Heinrich-Heine-Universität Düsseldorf, University of the Witwatersrand, and Ben-Gurion University of the Negev. The image depicts Ti vacancies in TiO as powerful drivers of photo- and photo-electrocatalytic seawater splitting for hydrogen production. Read the full text of the article at 10.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2021
The salts {[Ln Ln*(Hhmq) (OAc) (hfac) ] [Ln*(hfac) (OAc)(MeOH)] } (Hhmq=2-methanolquinolin-8-oxide, hfac=hexafluoroacetylacetonate; Ln, Ln*=Er, Gd, Yb) feature a discrete heteronuclear cation consisting of two types of lanthanide atoms. The quinolinoxy O-atom serves as a μ -bridge to two Ln atoms and as a μ -bridge to all three atoms, with metal⋅⋅⋅metal distances being around 3.7 Å.
View Article and Find Full Text PDFPhotodriven seawater splitting is considered to be one of the most promising techniques for sustainable hydrogen production. However, the high salinity of seawater would deactivate catalysts and consume the photogenerated carriers. Metal vacancies in metal oxide semiconductors are critical to directed electron transfer and high salinity resistance; they are thus desirable but remain a challenge.
View Article and Find Full Text PDFFractal Pt-based materials with hierarchical structures and high self-similarity have attracted more and more attention due to their bioinspiring maximum optimization of energy utilization and mass transfer. However, their high-efficiency design of the mass- and electron-transfer still remains to be a great challenge. Herein, fractal PtPdCu hollow sponges (denoted as PtPdCu-HS) facilitating both directed mass- and electron-transfer are presented.
View Article and Find Full Text PDFExploring excellent peroxidase mimics with enhanced peroxidase-like activity is important to the construction of a fast, low-cost, and convenient colorimetric sensing platform for heavy ions. In this work, 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (HTCPP) was first used to modify ZnS/CoS and make it show better peroxidase-like activity. The metal-cation vacancies generated by Hg contacting HTCPP/ZnS/CoS further stimulate the catalytic activity.
View Article and Find Full Text PDFA highly efficient photoenergy conversion is strongly dependent on the cumulative cascade efficiency of the photogenerated carriers. Spatial heterojunctions are critical to directed charge transfer and, thus, attractive but still a challenge. Here, a spatially ternary titanium-defected TiO@carbon quantum dots@reduced graphene oxide (denoted as @CQDs@rGO) in one system is shown to demonstrate a cascade effect of charges and significant performances regarding the photocurrent, the apparent quantum yield, and photocatalysis such as H production from water splitting and CO reduction.
View Article and Find Full Text PDFHierarchical porosity and functionalization help to fully make use of metal-organic frameworks (MOFs) for their diverse applications. Herein, a simple strategy is reported to construct hierarchically porous MOFs through a competitive coordination method using tetrafluoroborate (M(BF ) , where M is metal site) as both functional sites and etching agents. The resulting MOFs have in situ formed defect-mesopores and functional sites without sacrificing their structure stability.
View Article and Find Full Text PDFFlexible organic solar cells (OSCs) are considered one key component in wearable, intelligent electronics due to the unique capacity for highly flexible renewable energy sources. However, it is urgently required to enhance their efficiency, as it is far inferior to that of their conventional, glass-based counterparts. To boost the performance of flexible OSCs on plastic substrates, we here present a synergetic transparent electrode structure, which combines electrically conductive silver nanowires, a sol-gel-derived ZnO planarization layer, and imprinted light-trapping nanostructures.
View Article and Find Full Text PDFThe homojunction of oxygen/metal vacancies and its interfacial n-p effect on the physiochemical properties are rarely reported. Interfacial n-p homojunctions of TiO are fabricated by directly decorating interfacial p-type titanium-defected TiO around n-type oxygen-defected TiO nanocrystals in amorphous-anatase homogeneous nanostructures. Experimental measurements and theoretical calculations on the cell lattice parameters show that the homojunction of oxygen and titanium vacancies changes the charge density of TiO ; a strong EPR signal caused by oxygen vacancies and an unreported strong titanium vacancies signal of 2D H TQ-SQ MAS NMR are present.
View Article and Find Full Text PDFRapid progress in the power conversion efficiency (PCE) of polymer solar cells (PSEs) is beneficial from the factors that match the irradiated solar spectrum, maximize incident light absorption, and reduce photogenerated charge recombination. To optimize the device efficiency, a nanopatterned ZnO:Al O composite film is presented as an efficient light- and charge-manipulation layer (LCML). The Al O shells on the ZnO nanoparticles offer the passivation effect that allows optimal electron collection by suppressing charge-recombination loss.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2016
The assembly sequence of the coordination cluster [Zn5 (H2 L(n) )6 ](NO3 )4 ]⋅8 H2 O⋅2 CH3 OH (Zn5 , H3 L(n) =(1,2-bis(benzo[d]imidazol-2-yl)-ethenol) involves in situ dehydration of 1,2-bis(benzo[d]imidazol-2-yl)-1,2-ethanediol (H4 L) through the formation of the [Zn(H3 L)2 ](+) monomer, dimerization to [Zn2 (H3 L)2 ](+) , dehydration of the ligand to [Zn2 (H2 L(n) )2 ](+) , and the final formation of the pentanuclear cluster. The cluster has the following special characteristics: 1) high stability in both refluxing 37 % HCl and 27 % NH3 , 2) low cytotoxicity, and 3) pH-sensitive fluorescence in the visible-to-near-infrared (Vis/NIR) region in the solid state and in solution. We have applied it as a fluorescent probe both in vivo and in vitro.
View Article and Find Full Text PDF