Quasi-homogeneous photoelectrochemical organic transformations for tunable products and 100%conversion ratio

Photoelectrochemical(PEC)organic transformation at the anode coupled with cathodic H_(2) generation is a potentially rewarding strategy for efficient solar energy utilization.Nevertheless,achieving the full conversion of organic substrates with exceptional product selectivity remains a formidable hurdle in the context of heterogeneous catalysis at the solid/liquid interface.Here,we put forward a quasi-homogeneous catalysis concept by using the reactive oxygen species(ROS),such as·OH,H_(2)O_(2) and SO_(4)^(2-),as a charge transfer mediator instead of direct heterogeneous catalysis at the solid/liquid interface.In the context of glycerol oxidation,all ROS exhibited a preference forfirst-order reaction kinetics.These ROS,however,showcased distinct oxidation mechanisms,offering a range of advantages such as100%conversion ratios and theflexibility to tune the resulting products.Glycerol oxidative formic acid with Faradaic efficiency(FE)of 81.2%was realized by the H_(2)O_(2) and·OH,while SO_(4)^(2-)was preferably for glycerol conversion to C3 products like glyceraldehyde and dihydroxyacetone with a total FE of about 80%.Strikingly,the oxidative coupling of methane to ethanol was successfully achieved in our quasi-homogeneous system,yielding a remarkable production rate of 12.27 lmol h^(-1) and an impressive selectivity of 92.7%.This study is anticipated to pave the way for novel approaches in steering solar-driven organic conversions by manipulating ROS to attain desired products and conversion ratios.

Erratum to: Low-intensity pulsed ultrasound ameliorates angiotensin II-induced cardiac fibrosis by alleviating inflammation via a caveolin-1-dependent pathway

The original version of this article(Zhao et al.,2021)unfortunately contained two mistakes.(1)In p.826,the hematoxylin eosin(HE)staining figure of the fourth panel(the Ang Ⅱ+LIPUS group)in Fig.3a was incorrect.

Direct photoelectrochemical nitrate synthesis in an acidic electrolyte from N_(2)by a hole coupled oxygen atom transfer process

Ammonia is an important chemical for pharmaceutical,agriculture,industry,as well as energy production et al.However,the industrial production of ammonia using the Haber-Bosch process is energy-intensive,which stimulates us to explore a cost-effective and low-carbon footprint way for the synthesis of ammonia[1–3].Electrochemical(EC)synthesis of ammonia from an aqueous N_(2)reduction reaction(NRR)has gained significant attention in recent years,while the high dissociation energy of the N≡N bond(941 kJ/mol),as well as higher over-potential than hydrogen evolution reaction(HER),cause a lower efficiency[4].

Low‐intensity pulsed ultrasound ameliorates angiotensin II-induced cardiac fibrosis by alleviating inflammation via a caveolin-1-dependent pathway

Objective:Cardiac hypertrophy and fibrosis are major pathological manifestations observed in left ventricular remodeling induced by angiotensin II(AngII).Low-intensity pulsed ultrasound(LIPUS)has been reported to ameliorate cardiac dysfunction and myocardial fibrosis in myocardial infarction(MI)through mechano-transduction and its downstream pathways.In this study,we aimed to investigate whether LIPUS could exert a protective effect by ameliorating AngII-induced cardiac hypertrophy and fibrosis and if so,to further elucidate the underlying molecular mechanisms.Methods:We used AngII to mimic animal and cell culture models of cardiac hypertrophy and fibrosis.LIPUS irradiation was applied in vivo for 20 min every 2 d from one week before mini-pump implantation to four weeks after mini-pump implantation,and in vitro for 20 min on each of two occasions 6 h apart.Cardiac hypertrophy and fibrosis levels were then evaluated by echocardiographic,histopathological,and molecular biological methods.Results:Our results showed that LIPUS could ameliorate left ventricular remodeling in vivo and cardiac fibrosis in vitro by reducing AngII-induced release of inflammatory cytokines,but the protective effects on cardiac hypertrophy were limited in vitro.Given that LIPUS increased the expression of caveolin-1 in response to mechanical stimulation,we inhibited caveolin-1 activity with pyrazolopyrimidine 2(pp2)in vivo and in vitro.LIPUS-induced downregulation of inflammation was reversed and the anti-fibrotic effects of LIPUS were absent.Conclusions:These results indicated that LIPUS could ameliorate AngII-induced cardiac fibrosis by alleviating inflammation via a caveolin-1-dependent pathway,providing new insights for the development of novel therapeutic apparatus in clinical practice.

酰胺功能化共价三嗪骨架增强光催化析氢

具有富氮共轭骨架的共价三嗪骨架(CTFs)是一类典型的共价有机骨架(COFs)多孔材料,因其优异的化学和物理稳定性、结构可调性和低骨架密度等特性,在光催化氧化还原反应研究方面逐渐受到重视.与众多COFs材料一样,CTFs的光催化活性与材料的结晶性和官能团修饰密切相关.然而,CTFs的合成途径较为单一,主要通过强有机酸催化氰基不可逆热聚合,以致CTFs较难通过结晶和官能团修饰协同提升催化活性.在本工作中,我们发现CF_(3)SO_(3)H催化热聚合制备的CTF-1具有很高的结晶度且晶粒表面含有大量未反应的氰基.将CTF-1浸没在盐酸溶液中,通过超声辅助促使表面氰基水解成酰胺基团,获得了酰胺功能化的高结晶性CTFs(CTF-amide).研究表明,随着盐酸处理时间的增加,更多的氰基转化为酰胺基团,相应材料的光催化活性增强越明显.其中CTF-amide-16的光催化分解水析氢速率为1133μmol g^(-1)h^(-1),远高于原始的CTF-1(520μmol g^(-1)h^(-1)).电化学和瞬态吸收结果表明,酰胺基团功能化有利于CTF中光生载流子的分离和迁移.