Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.

Ultrathin origami accordion-like structure of vacancy-rich graphitized carbon nitride for enhancing CO_(2) photoreduction

Retaining the ultrathin structure of two-dimensional materials is very important for stabilizing their catalytic performances.However,aggregation and restacking are unavoidable,to some extent,due to the van der Waals interlayer interaction of two-dimensional materials.Here,we address this challenge by preparing an origami accordion structure of ultrathin twodimensional graphitized carbon nitride(oa-C_(3)N_(4))with rich vacancies.This novel structured oa-C_(3)N_(4) shows exceptional photocatalytic activity for the CO_(2) reduction reaction,which is 8.1 times that of the pristine C_(3)N_(4).The unique structure not only prevents restacking but also increases light harvesting and the density of vacancy defects,which leads to modification of the electronic structure,regulation of the CO_(2) adsorption energy,and a decrease in the energy barrier of the carbon dioxide to carboxylic acid intermediate reaction.This study provides a new avenue for the development of stable highperformance two-dimensional catalytic materials.

Outer delocalized electron aggregation of bromide bridged core–shell CuBr@C for hydrogen evolution reaction

Modulation of the surface electron distribution is a challenging problem that determines the adsorption ability of catalytic process.Here,we address this challenge by bridging the inner and outer layers of the core–shell structure through the bridge Br atom.Carbon shell wrapped copper bromide nanorods(CuBr@C)are constructed for the first time by chemical vapour deposition with hexabromobenzene(HBB).HBB pyrolysis provides both bridge Br atom and C shells.The C shell protects the stability of the internal halide structure,while the bridge Br atom triggers the rearrangement of the surface electrons and exhibits excellent electrocatalytic activity.Impressively,the hydrogen evolution reaction(HER)activity of CuBr@C is significantly better than that of commercial N-doped carbon nanotubes,surpassing commercial Pt/C at over 200 mA·cm^(−2).Density functional theory(DFT)calculations reveal that bridge Br atoms inspire aggregation of delocalized electrons on C-shell surfaces,leading to optimization of hydrogen adsorption energy.

Association of Renin Binding Protein(RnBP) Gene Polymorphisms with Essential Hypertension in the Hani Minority of Southwestern China

Essential hypertension is one of the most common multi- factorial diseases, affecting 20%--30% of the human popula- tion （Ibrahim and Damasceno, 2012）. Based on the results of twin studies, adoption studies and statistical analyses of blood pressure （BP） across various pedigrees, it has been estimated that 30%--50% of the variability in blood pressure among the general population is genetically determined （Garcia et al., 2003）. Although the genetic mechanisms of essential hyper- tension have not been studied well, investigations for the genes that constitute the renin-angiotensin system （RAS） appear to be particularly promising, since this system plays a central role in the regulation of blood pressure （Ferrario, 2010）.