Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term a...Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term and large-scale implementation of electrochemical CO_(2) reduction technology is the lack of active and selective cat-alysts.Copper(Cu)is one of the few candidates that can facilitate C–C coupling to obtain high-energy oxygenates and hydrocarbons beyond carbon monoxide(CO),but it suffers from poor selectivity for products of interest and high overpotentials.Alloying is an effective way to break the linear scaling relations and uniquely manipulate the reactivity and selectivity,which is hard to achieve by using monometallic compositions alone.By alloying Cu with other metals,one could change the catalytic properties of the catalyst by tuning the local electronic structure and modulating the adsorption strength of the reaction intermediates,thus improving the catalytic activity and selectivity.In this review,we focus on the recently developed Cu-based alloy catalysts(including conventional alloys,high-entropy alloys and single-atom alloys)that have been applied in electrocatalytic CO_(2) reduction(ECR).Theoretical calculations and experimental advances in understanding the key rate-limiting and selectivity-determining steps in those alloys are summarized,with a particular focus on identifying binding energy de-scriptors and the dynamic product formation mechanisms.In addition,we outline the opportunities and chal-lenges in the fundamental understanding of ECR by recommending advanced in-situ characterization techniques and standardized electrochemical methods and offer atomic-level design principles for steering the reaction pathways to the desired products.展开更多
To improve the diagnostic efficiency of prostate cancer(PCa)and reduce unnecessary biopsies,we defined and analyzed the diagnostic efficiency of peripheral zone prostate-specific antigen(PSA)density(PZ-PSAD).Patients ...To improve the diagnostic efficiency of prostate cancer(PCa)and reduce unnecessary biopsies,we defined and analyzed the diagnostic efficiency of peripheral zone prostate-specific antigen(PSA)density(PZ-PSAD).Patients who underwent systematic 12-core prostate biopsies in Shanghai General Hospital(Shanghai,China)between January 2012 and January 2018 were retrospectively identified(n=529).Another group of patients with benign prostatic hyperplasia(n=100)were randomly preselected to obtain the PSA density of the non-PCa cohort(N-PSAD).Prostate volumes and transition zone volumes were measured using multiparameter magnetic resonance imaging(mpMRI)and were combined with PSA and N-PSAD to obtain the PZ-PSAD from a specific algorithm.Receiver operating characteristic(ROC)curve analysis was used to assess the PCa detection efficiency in patients stratified by PSA level,and the area under the ROC curve(AUC)of PZ-PSAD was higher than that of PSA,PSA density(PSAD),and transition zone PSA density(TZ-PSAD).PZ-PSAD could amend the diagnosis for more than half of the patients with inaccurate transrectal ultrasonography(TRUS)and mpMRI results.When TRUS and mpMRI findings were ambiguous to predict PCa(PIRADS score≤3),PZ-PSAD could increase the positive rate of biopsy from 21.7%to 54.7%,and help 63.8%(150/235)of patients avoid unnecessary prostate biopsy.In patients whose PSA was 4.0–10.0 ng ml^(−1),10.1–20.0 ng ml^(−1),and>20.0 ng ml^(−1),the ideal PZ-PSAD cut-off value for predicting clinically significant PCa was 0.019 ng ml^(−2),0.297 ng ml^(−2),and 1.180 ng ml^(−2),respectively(sensitivity>90%).Compared with PSA,PSAD,and TZ-PSAD,the efficiency of PZ-PSAD for predicting PCa is the highest,leading to fewer missed diagnoses and unnecessary biopsies.展开更多
基金the National Natural Science Foundation of China(NSFC 22102018 and 52171201)the Natural Science Foundation of Sichuan Province(2022NSFSC0194)+6 种基金the Central Government Funds of Guiding Local Scientific and Technological Development for Sichuan Province(2021ZYD0043)the University of Electronic Science and Technology of China for Startup Funding(A1098531023601264)the Hefei National Research Center for Physical Sciences at the Micro-scale(KF2021005)the China Postdoctoral Science Foundation funded project(2022M710601)the University of Elec-tronic Science and Technology of China for Startup Funding(Y030212059003039)the NSFC(22005291 and 22278067)University of Electronic Science and Technology of China for Startup Funding(A1098531023601356).
文摘Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term and large-scale implementation of electrochemical CO_(2) reduction technology is the lack of active and selective cat-alysts.Copper(Cu)is one of the few candidates that can facilitate C–C coupling to obtain high-energy oxygenates and hydrocarbons beyond carbon monoxide(CO),but it suffers from poor selectivity for products of interest and high overpotentials.Alloying is an effective way to break the linear scaling relations and uniquely manipulate the reactivity and selectivity,which is hard to achieve by using monometallic compositions alone.By alloying Cu with other metals,one could change the catalytic properties of the catalyst by tuning the local electronic structure and modulating the adsorption strength of the reaction intermediates,thus improving the catalytic activity and selectivity.In this review,we focus on the recently developed Cu-based alloy catalysts(including conventional alloys,high-entropy alloys and single-atom alloys)that have been applied in electrocatalytic CO_(2) reduction(ECR).Theoretical calculations and experimental advances in understanding the key rate-limiting and selectivity-determining steps in those alloys are summarized,with a particular focus on identifying binding energy de-scriptors and the dynamic product formation mechanisms.In addition,we outline the opportunities and chal-lenges in the fundamental understanding of ECR by recommending advanced in-situ characterization techniques and standardized electrochemical methods and offer atomic-level design principles for steering the reaction pathways to the desired products.
基金This study was supported by the National Natural Science Foundation of China(No.81772746,No.81870516)Natural Science Foundation of Xinjiang Province(2019D01C091).
文摘To improve the diagnostic efficiency of prostate cancer(PCa)and reduce unnecessary biopsies,we defined and analyzed the diagnostic efficiency of peripheral zone prostate-specific antigen(PSA)density(PZ-PSAD).Patients who underwent systematic 12-core prostate biopsies in Shanghai General Hospital(Shanghai,China)between January 2012 and January 2018 were retrospectively identified(n=529).Another group of patients with benign prostatic hyperplasia(n=100)were randomly preselected to obtain the PSA density of the non-PCa cohort(N-PSAD).Prostate volumes and transition zone volumes were measured using multiparameter magnetic resonance imaging(mpMRI)and were combined with PSA and N-PSAD to obtain the PZ-PSAD from a specific algorithm.Receiver operating characteristic(ROC)curve analysis was used to assess the PCa detection efficiency in patients stratified by PSA level,and the area under the ROC curve(AUC)of PZ-PSAD was higher than that of PSA,PSA density(PSAD),and transition zone PSA density(TZ-PSAD).PZ-PSAD could amend the diagnosis for more than half of the patients with inaccurate transrectal ultrasonography(TRUS)and mpMRI results.When TRUS and mpMRI findings were ambiguous to predict PCa(PIRADS score≤3),PZ-PSAD could increase the positive rate of biopsy from 21.7%to 54.7%,and help 63.8%(150/235)of patients avoid unnecessary prostate biopsy.In patients whose PSA was 4.0–10.0 ng ml^(−1),10.1–20.0 ng ml^(−1),and>20.0 ng ml^(−1),the ideal PZ-PSAD cut-off value for predicting clinically significant PCa was 0.019 ng ml^(−2),0.297 ng ml^(−2),and 1.180 ng ml^(−2),respectively(sensitivity>90%).Compared with PSA,PSAD,and TZ-PSAD,the efficiency of PZ-PSAD for predicting PCa is the highest,leading to fewer missed diagnoses and unnecessary biopsies.
