Electrocatalytic NO reduction reaction to generate NH_(3)under ambient conditions offers an attractive alternative to the energy-extensive Haber-Bosch route;however,the challenge still lies in the development of cost-...Electrocatalytic NO reduction reaction to generate NH_(3)under ambient conditions offers an attractive alternative to the energy-extensive Haber-Bosch route;however,the challenge still lies in the development of cost-effective and high-performance electrocatalysts.Herein,nanoporous VN film is first designed as a highly selective and stable electrocatalyst for catalyzing reduction of NO to NH_(3)with a maximal Faradaic efficiency of 85%and a peak yield rate of 1.05×10^(-7)mol·cm^(-2)·s^(-1)(corresponding to 5,140.8mg·h^(-1)·mg_(cat).^(-1))at-0.6 V vs.reversible hydrogen electrode in acid medium.Meanwhile,this catalyst maintains an excellent activity with negligible current density and NH_(3)yield rate decays over 40 h.Moreover,as a proof-of-concept of Zn-NO battery,it delivers a high power density of 2.0 mW·cm^(-2)and a large NH_(3)yield rate of 0.22×10^(-7)mol·cm^(-2)·s^(-1)(corresponding to 1,077.1mg·h^(-1)·mg_(cat).^(-1)),both of which are comparable to the best-reported results.Theoretical analyses confirm that the VN surface favors the activation and hydrogenation of NO by suppressing the hydrogen evolution.This work highlights that the electrochemical NO reduction is an eco-friendly and energy-efficient strategy to produce NH_(3).展开更多
Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention.Herein we construct the well-defined Mn single-atom(MnSA)catalyst with four N-c...Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention.Herein we construct the well-defined Mn single-atom(MnSA)catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions(CO_(2)RR)and oxygen reduction reactions(ORR).MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90%at-0.9 V for CO_(2)RR and higher H_(2)O_(2)yield from 0.1 to 0.6 V with excellent ORR activity.Density functional theory(DFT)calculations based on constant potential models were performed to study the mechanism of MnSA on CO_(2)RR.The thermodynamic energy barrier of CO_(2)RR is lowest at-0.9 V vs.reversible hydrogen electrode(RHE).Similar DFT calculations on the H_(2)O_(2)yield of ORR showed that the H_(2)O_(2)yield at 0.2 V was higher.This study provides a reasonable explanation for the role of electrode potential micro-environments.展开更多
Human microorganisms,including bacteria,fungi,and viruses,play key roles in several physiological and pathological processes.Some studies discovered that tumour tissues once considered sterile actually host a variety ...Human microorganisms,including bacteria,fungi,and viruses,play key roles in several physiological and pathological processes.Some studies discovered that tumour tissues once considered sterile actually host a variety of microorganisms,which have been confirmed to be closely related to oncogenesis.The concept of intratumoural microbiota was subsequently proposed.Microbiota could colonise tumour tissues through mucosal destruction,adjacent tissue migration,and hematogenic invasion and affect the biological behaviour of tumours as an important part of the tumour microenvironment.Mechanistic studies have demonstrated that intratumoural microbiota potentially promote the initiation and progression of tumours by inducing genomic instability and mutations,affecting epigenetic modifications,promoting inflammation response,avoiding immune destruction,regulating metabolism,and activating invasion and metastasis.Since more comprehensive and profound insights about intratumoral microbiota are continuously emerging,new methods for the early diagnosis and prognostic assessment of cancer patients have been under examination.In addition,interventions based on intratumoural microbiota show great potential to open a new chapter in antitumour therapy,especially immunotherapy,although there are some inevitable challenges.Here,we aim to provide an extensive review of the concept,development history,potential sources,heterogeneity,and carcinogenic mechanisms of intratumoural microorganisms,explore the potential role of microorganisms in tumour prognosis,and discuss current antitumour treatment regimens that target intratumoural microorganisms and the research prospects and limitations in this field.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22075211,22109118,21601136,51971157,51621003,and 21905246)Tianjin Science Fund for Distinguished Young Scholars(No.19JCJQJC61800)The authors would also like to express their gratitude to Deanship of Scientific Research at King Khalid University,Abha,Saudi Arabia for funding this work through the Research Group Program under No.RGP.2/79/43.
文摘Electrocatalytic NO reduction reaction to generate NH_(3)under ambient conditions offers an attractive alternative to the energy-extensive Haber-Bosch route;however,the challenge still lies in the development of cost-effective and high-performance electrocatalysts.Herein,nanoporous VN film is first designed as a highly selective and stable electrocatalyst for catalyzing reduction of NO to NH_(3)with a maximal Faradaic efficiency of 85%and a peak yield rate of 1.05×10^(-7)mol·cm^(-2)·s^(-1)(corresponding to 5,140.8mg·h^(-1)·mg_(cat).^(-1))at-0.6 V vs.reversible hydrogen electrode in acid medium.Meanwhile,this catalyst maintains an excellent activity with negligible current density and NH_(3)yield rate decays over 40 h.Moreover,as a proof-of-concept of Zn-NO battery,it delivers a high power density of 2.0 mW·cm^(-2)and a large NH_(3)yield rate of 0.22×10^(-7)mol·cm^(-2)·s^(-1)(corresponding to 1,077.1mg·h^(-1)·mg_(cat).^(-1)),both of which are comparable to the best-reported results.Theoretical analyses confirm that the VN surface favors the activation and hydrogenation of NO by suppressing the hydrogen evolution.This work highlights that the electrochemical NO reduction is an eco-friendly and energy-efficient strategy to produce NH_(3).
基金supported by the National Natural Science Foundation of China(Nos.52073214 and 22075211)Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008).
文摘Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention.Herein we construct the well-defined Mn single-atom(MnSA)catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions(CO_(2)RR)and oxygen reduction reactions(ORR).MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90%at-0.9 V for CO_(2)RR and higher H_(2)O_(2)yield from 0.1 to 0.6 V with excellent ORR activity.Density functional theory(DFT)calculations based on constant potential models were performed to study the mechanism of MnSA on CO_(2)RR.The thermodynamic energy barrier of CO_(2)RR is lowest at-0.9 V vs.reversible hydrogen electrode(RHE).Similar DFT calculations on the H_(2)O_(2)yield of ORR showed that the H_(2)O_(2)yield at 0.2 V was higher.This study provides a reasonable explanation for the role of electrode potential micro-environments.
基金supported by the National Natural Science Foundation of China(No.82330003,No.82070099,No.82102496,No.82001988)National Science and Technology Major Project of the Ministry of Science and Technology of China(2022YFF1203300)+1 种基金Major Project of the Department of Science and Technology of Hubei(2022BCA016)Hubei Key Laboratory of Biological Targeted Therapy(2022swbx009).
文摘Human microorganisms,including bacteria,fungi,and viruses,play key roles in several physiological and pathological processes.Some studies discovered that tumour tissues once considered sterile actually host a variety of microorganisms,which have been confirmed to be closely related to oncogenesis.The concept of intratumoural microbiota was subsequently proposed.Microbiota could colonise tumour tissues through mucosal destruction,adjacent tissue migration,and hematogenic invasion and affect the biological behaviour of tumours as an important part of the tumour microenvironment.Mechanistic studies have demonstrated that intratumoural microbiota potentially promote the initiation and progression of tumours by inducing genomic instability and mutations,affecting epigenetic modifications,promoting inflammation response,avoiding immune destruction,regulating metabolism,and activating invasion and metastasis.Since more comprehensive and profound insights about intratumoral microbiota are continuously emerging,new methods for the early diagnosis and prognostic assessment of cancer patients have been under examination.In addition,interventions based on intratumoural microbiota show great potential to open a new chapter in antitumour therapy,especially immunotherapy,although there are some inevitable challenges.Here,we aim to provide an extensive review of the concept,development history,potential sources,heterogeneity,and carcinogenic mechanisms of intratumoural microorganisms,explore the potential role of microorganisms in tumour prognosis,and discuss current antitumour treatment regimens that target intratumoural microorganisms and the research prospects and limitations in this field.
