CO2 electrolysis at industrial current densities using anion exchange membrane based electrolyzers

Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.

Remarkable difference of phospholipid molecular chirality in regulating PrP aggregation and cell responses

Prion diseases are fatal neurodegenerative diseases that can cause severe dementia.The misfolding and accumulation of the prion peptide (PrP)_(106–126) is crucial,and this process is closely relevant to biological membranes.However,how PrP_(106–126)aggregation is affected by the molecular chirality of phospholipid membrane is unknown.Thus,in this study,a pair of L-and D-aspartic acid (Asp)-modified 1,2-dipalmitoyl-sn–glycero-3-phosphoethanolamine (DPPE) were synthesized to construct chiral liposomes.We discover that L-Asp-DPPE liposomes strongly inhibit the oligomerization and amyloidogenesis of PrP_(106–126),whether acting on monomers or oligomers,which rescues cytotoxicity induced by PrP_(106–126).By comparison,D-Asp-DPPE liposomes inhibit peptide oligomerization only at a high concentration and cannot prevent amyloidogenesis when acting on oligomers,which lead to pronounced cytotoxicity.Apoptosis experiment,dynamic change of intracellular Ca^(2+)(_(i)Ca^(2+)) and Ca^(2+)release from endoplasmic reticulum(ER),reactive oxygen species (ROS) production,adsorption dynamics and affinity tests,and fluorescent imaging clearly disclose that molecular chirality of the liposomes dominates conformational transition of PrP_(106–126)from random coil to β-sheet,binding and adsorption of the monomers and oligomers,and subsequent fibrillation process,resulting in distinct inhibition effect in Ca^(2+)overload and release,ROS production and cell apoptosis.This work is the first to report that interfacial molecular chirality is a potentially crucial influence on the fibrillation process of PrP_(106–126) and its cell responses,whereas the convergence of chiral amino acids and liposomes can be considered potential inhibitors in prion diseases.

Self-assembly of phosphorylated peptide driven by Dy^(3+)

Nature chooses phosphorylation as a key modification to modulate and program the functions of proteins.Various phosphorylated peptides(PPs)have been widely identified and investigated by biologists,but the possibility that PPs could become a building unit for artificial materials is neglected.Here we report for the first time a supramolecular assembly of PPs with the assistance of dysprosium ions(Dy^(3+)).Dy^(3+)bridges multiple phosphate groups in double-phosphorylated peptides(di-PPs),and braid these peptide chains into nanofibers.The assembly occurs inside nanochannels and blocks the channels,leading to prominent“ON–OFF”switching in transmembrane ionic current.The di-PPs’assembling process could be dynamically regulated by the addition or deletion of phosphate groups under the control of kinases or phosphatases.This study proves the huge potential of PPs being utilized as materials via self-assembling,which will promote the design of novel bio-inspired artificial materials and devices.

Sensing Mechanism of Excited-State Intermolecular Hydrogen Bond for Phthalimide: Indispensable Role of Dimethyl Sulfoxide

Excited-state hydrogen bond strongly affects the intramolecular charge conversion process,which is very suitable for the design and development of high-performance fluorescent probes.However,as one of the most common solvents or additives used in sensing,the role of dimethyl sulfoxide(DMSO)in the system of the excited-state hydrogen bond is seldom explored.As the goal of this research,we investigated the sensing mechanism of a C0RM3-green fluorescent probe system for carbon monoxide releasing molecule(CORM-3)detection and tracking in vivo,through quantum chemistry calculations based on density-functional-theory(DFT)/time-dependent density-functional-theory(TDDFT)methods.Based on the analysis of the solvent effect of DMSO by the reduced density gradient function and IR spectroscopy,we provided a new strategy to explain the fluorescence mechanism.Subsequently,we verified the result through the potential energy curve of Phthalimide(PTI,the reduced product of C0RM3-green).The excited-state hydrogen bond between PTI and DMSO promotes radiation transition and leads to obvious difference in the photophysical properties of PTI and PTI-DMSO.

Label-Free,Versatile,Real-Time,and High-Throughput Monitoring of Tyrosine Phosphorylation Based on Reversible Configuration Freeze

Tyrosine Phosphorylation(pTyr)is a critical and ubiquitous regulation mechanism in biology that plays a central role in controlling intracellular signaling networks.Precise recognition and specific detection of pTyr peptides have been of great importance for both discoveries of disease biomarkers and screening of therapeutic drugs,especially cancers.Here we report a label-free,versatile,realtime,and high-throughput detection strategy for phosphopeptide(PP)based on reversible configuration freeze of a unique hemicyanine-labeled 2-(2′-hydroxyphenyl)-4-methyloxazole(H-HPMO).By taking advantage of the“OFF–ON”transition of fluorescence,H-HPMO–Cu^(2+)complex displays a highly sensitive and selective response to PPs with modified sites on serine,threonine,and tyrosine.Specific recognition of Tyr PPs is achieved by performing a simple logic gate operation and introducing Ca^(2+)interference as an input.This PP detection approach is universal for various peptide sequences and displays high potential in large-scale kinase inhibitor screening,which will promote the development of targeted anticancer drugs.

Unique three-component co-assembly among AIEgen,L-GSH,and Ag^(+)for the formation of helical nanowires

Nature has selected,produced,and evolved numerous molecular architectural motifs over billions of years for particular bio-functions.During this process,molecular self-assembly plays a critically important role.Inspired by these delicate assemblies,scientists devote themselves to developing various sophisticated complexes assembled by diverse and numerous structural motifs.By far,most of the examples focus on single-molecule self-assembly or co-assembly between two molecules,seldom works report the co-assembly among three building blocks due to the substantially increased complexity and decreased controllability.Here we report a novel three-component co-assembly among L-glutathione(L-GSH),AgNO_(3),and an aggregation-induced emission luminogen(AIEgen),namely triphenylamine-pyridinium(abbreviated to TPA-Py).TPA-Py,L-GSH,and Ag^(+)co-assemble into numerous long and ordered nanowires with left-handed helices,which show remarkable AIE properties that can be observed by naked eyes.This effect is only detected in this system,the replacement of TPA-Py with other AIEgens,L-GSH with other cysteine derivatives or anions,Ag^(+)with other metal ions,could not lead to the unique AIE effect,which endows this system with high specificity and controllability.This work provides new insight into the design of biomolecule recognition systems and discloses that ternary co-assembly could become a facile route to build sophisticated nanobiomaterials.