Switching CO2 Electroreduction toward Ethanol by Delocalization State-Tuned Bond Cleavage.

The electrochemical CO2 reduction reaction by copper-based catalysts features a promising approach to generate value-added multicarbon (C2+) products. However, due to the unfavored formation of oxygenate intermediates on the catalyst surface, the selectivity of C2+ alcohols like ethanol remains unsatisfactory compared to that of ethylene. The bifurcation point (i.e., the CH2═CHO* intermediate adsorbed on Cu via a Cu-O-C linkage) is critical to the C2+ product selectivity, whereas the subsequent cleavage of the Cu-O or the O-C bond determines the ethanol or ethylene pathway. Inspired by the hard-soft acid-base theory, in this work, we demonstrate an electron delocalization tuning strategy of the Cu catalyst by a nitrene surface functionalization approach, which allows weakening and cleaving of the Cu-O bond of the adsorbed CH2═CHO*, as well as accelerating hydrogenation of the C═C bond along the ethanol pathway. As a result, the nitrene-functionalized Cu catalyst exhibited a much-enhanced ethanol Faradaic efficiency of 45% with a peak partial current density of 406 mA·cm-2, substantially exceeding that of unmodified Cu or amide-functionalized Cu. When assembled in a membrane electrode assembly electrolyzer, the catalyst presented a stable CO2-to-ethanol conversion for >300 h at an industrial current density of 400 mA·cm-2.

Hydrophobic Composite Foams with Asymmetric Gradient Sandwich Structure for Excellent Electromagnetic Interference Shielding and Photothermal Response.

The evolution of contemporary electronics urgently requires the use of versatile electromagnetic interference (EMI) shielding materials in complex environments. Interlayer polydimethylsiloxane (PDMS)/Fe3O4@multiwalled carbon nanotubes (MWCNTs) foams were prepared by a simple physical foaming method with excellent flexibility and electromagnetic wave absorption. The bottom nickel aramid paper (NiP) layer creates a dense conductive network by chemical plating technology, which ensures excellent EMI effectiveness. The upper carbon black (CB)/Fe3O4 layer further improves the absorption performance via conductive loss and magnetic loss. With the effective layout of the impedance matching layer, absorbing layer, and conductive shielding layer, the CB/Fe3O4-PDMS/Fe3O4@MWCNTs-NiP composite material achieves an EMI shielding effectiveness (EMI SE) of 61.7 dB and an absorption coefficient of 0.58 at X-band. In addition, the composite foam provides photothermal conversion and hydrophobicity due to the effective stacking of PDMS and CB/Fe3O4. Thus, the multifunctional composite foam presents a broad range of possible applications, benefiting EMI shielding as well as other specific areas.

Interfacial Water Tuning by Intermolecular Spacing for Stable CO2 Electroreduction to C2+ Products.

Electroreduction of CO2 to multi-carbon (C2+ ) products is a promising approach for utilization of renewable energy, in which the interfacial water quantity is critical for both the C2+ product selectivity and the stability of Cu-based electrocatalytic sites. Functionalization of long-chain alkyl molecules on a catalyst surface can help to increase its stability, while it also tends to block the transport of water, thus inhibiting the C2+ product formation. Herein, we demonstrate the fine tuning of interfacial water by surface assembly of toluene on Cu nanosheets, allowing for sustained and enriched CO2 supply but retarded water transfer to catalytic surface. Compared to bare Cu with fast cathodic corrosion and long-chain alkyl-modified Cu with main CO product, the toluene assembly on Cu nanosheet surface enabled a high Faradaic efficiency of 78 % for C2+ and a partial current density of 1.81 A cm-2 . The toluene-modified Cu catalyst further exhibited highly stable CO2 -to-C2 H4 conversion of 400 h in a membrane-electrode-assembly electrolyzer, suggesting the attractive feature for both efficient C2+ selectivity and excellent stability.

Constructing high sensitivity thermometry with dual-emitting Nd3+/Er3+/Yb3+ codoped BaWO4 single crystal material.

Inorganic oxides doped with rear earth(RE) have attracted much interest because of their outstanding optical properties. In this paper, the BaWO4:Yb3+/Er3+/Nd3+ phosphors were successfully prepared by typical solid state method. The crystalline structure of the samples was characterized through X-ray diffraction(XRD). The morphology of that was demonstrated with field emission scanning electron microscopy(FE-SEM). Under 980 nm excitation, the BaWO4: Yb3+/Er3+/Nd3+ phosphor presented four typical emissions at green(524-550 nm, Er3+), red(∼655 nm, Er3+), near infrared(∼710 nm, ∼820 nm, Nd3+). Furthermore, the temperature sensing properties of the samples were investigated in the temperature range of 303-573 K. The fluorescence intensity ratio(FIR) technique based on thermal and non-thermal coupled levels was applied to analyse the sensing performances. For BaWO4:Yb3+/Er3+/Nd3+ phosphor, the maximum absolute sensitivity reached 0.0423 K-1 at 303 K, which is based on 2H11/2(Er3+) and 4F7/2(Nd3+) levels. The repeatability of temperature response also was proved through four cold and heat cycles. The above result indicated that the BaWO4:Yb3+/Er3+/Nd3+ phosphor would be a promising temperature sensing materials.

Efficient upconversion emission and high-sensitivity thermometry of BaIn2O4:Yb3+/Tm3+/RE3+ (RE = Er3+, Ho3+) phosphor.

BaIn2O4:Yb3+/Tm3+/RE3+ (RE = Er3+, Ho3+) upconversion (UC) phosphors were synthesized via the sol-gel method. Rietveld refinement based on XRD data proved that In3+ ions were replaced by rare earth (RE) ions. Under 980 nm excitation, UC and optical temperature-sensing properties were investigated, and the results indicated that the samples demonstrated high UC emission efficiencies and bright emission visible to the naked eye. The luminescence intensity ratio (LIR) technology based on thermally and non-thermally coupled levels was applied to study the optical temperature-sensing properties of the RE-doped BaIn2O4 phosphors. For the BaIn2O4:Yb3+/Tm3+/Er3+ phosphor, the absolute sensitivity reached a maximum value of 0.1433 K-1 at 473 K, which was based on the non-thermally coupled levels (non-TCLs) of 1G4 (blue luminescence at 480 nm of Tm3+ ion) and 2H11/2 (green luminescence at 525 nm of Er3+ ion). For the BaIn2O4:Yb3+/Tm3+/Ho3+ phosphor, the maximum absolute sensitivity was 0.2545 K-1, which came from the non-TCLs of 3H4 (infrared luminescence at 795 nm of Tm3+ ion) and 1G4 (blue luminescence at 480 nm of Tm3+ ion). BaIn2O4:Yb3+/Tm3+/RE3+ (RE = Er3+, Ho3+) samples were proven to have excellent optical temperature-sensing properties and could be applied to design optical thermometry.

Investigation on the upconversion luminescence and ratiometric thermal sensing of SrWO4:Yb3+/RE3+ (RE = Ho/Er) phosphors.

SrWO4 phosphors doped with Ho3+(Er3+)/Yb3+ are successfully prepared by a high temperature solid-state reaction method. The upconversion (UC) luminescence properties of all the samples have been investigated under 980 nm excitation. Strong green emissions are obtained in the SrWO4:Yb3+/Ho3+ and SrWO4:Yb3+/Er3+ samples with the naked eyes. In a temperature range going from 303 K to 573 K, the UC emission spectra of the phosphors have been measured. Then the temperature sensing properties also have been discussed via fluorescence intensity ratio (FIR) technology. For the SrWO4:Yb3+/Ho3+ phosphor, the FIR technologies based on thermal coupling levels (TCLs)(5F4,5F5) and non-thermal coupling levels (non-TCLs)(5S2, 5F4/5F5) are used for investigating the sensitivity. The results show that the maximum absolute sensitivity reaches 0.0158 K-1 with non-TCLs. As for Yb3+/Er3+ codoped SrWO4 phosphor, the maximum absolute sensitivity reaches 0.013 K-1 with TCLs (2H11/2,4S5/2) at a temperature of 513 K. These significant results demonstrate that the SrWO4:Ho3+(Er3+)/Yb3+ phosphors are robust for optical temperature sensors.

Genome-wide identification, characterisation and expression analysis of the ALAS gene in the Yesso scallop (Patinopecten yessoensis) with different shell colours.

Porphyrins, one of the most common shell pigments, are by-products of the haem pathway. 5-Aminolaevulinate synthase (ALAS) is the first and rate-limiting enzyme in this pathway and has been well studied in vertebrate species. However, the function of ALAS in shell colouration has been poorly studied in molluscs, which are renowned for their colourful shells. In the present study, an ALAS gene, named PyALAS, was identified through whole-genome scanning in the Yesso scallop (Patinopecten yessoensis), an economically and evolutionarily important bivalve species in which the shell colour represents polymorphism. Two conserved domains were detected in the PyALAS protein sequence, including a Preseq-ALAS domain and a 5-ALAS domain, confirming the identification of PyALAS. Phylogenetic analysis of the ALAS proteins among various invertebrate and vertebrate species revealed a high consistency between the molecular evolution of ALAS and the species taxonomy. PyALAS was ubiquitously expressed in most adult tissues of the Yesso scallop. The left mantle expressed a significantly higher level of PyALAS than the right side in brown scallops, whereas there was no significant difference in white scallops. Significantly different expression levels of PyALAS was also detected between the two different shell colour strains. These data indicate that PyALAS plays an important role in shell colouration in Yesso scallops and the present study provides new insights into the molecular mechanism of shell colouration in molluscs.

Effects of dietary supplementation of probiotic Shewanella colwelliana WA64, Shewanella olleyana WA65 on the innate immunity and disease resistance of abalone, Haliotis discus hannai Ino.

The effects of dietary administration of two probiotics, Shewanella colwelliana WA64 and Shewanella olleyana WA65, on the innate immunity of abalone (Haliotis discus hannai Ino), and survival of juvenile abalone challenged with Vibrio harveyi have been studied. Two groups of abalone were fed with three different diets: one control, and two diets supplemented with 10(9) cell g(-1) of probiotic WA64 (WA64 diet) and WA65 (WA65 diet) for up to four weeks. Results showed that abalone fed diets containing S. colwelliana WA64 and S. olleyana WA65 had led to an enhanced cellular and humoral immune response, notably higher haemocytes, respiratory burst activity, serum lysozyme activity and total protein levels were recorded after one week of probiotic administration. On the other hand, mortality after the challenges with V. harveyi in the group fed with control diet ranged from 77 to 80%, while mortality rates observed in the groups fed with diets supplemented with WA64 and WA65 ranged from 27 to 50% and 30-43%, respectively. The results demonstrated potential for S. colwelliana WA64 and S. olleyana WA65 to improve innate immunity and disease resistance in H. discus hannai.