The dynamic adsorption of possible intermediates on single-atom catalysts(SACs)under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction(OER),and therefore the perfo...The dynamic adsorption of possible intermediates on single-atom catalysts(SACs)under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction(OER),and therefore the performance of the dynamic adsorption should be fully considered in the theoretical screening of potential SACs.Based on density functional theory calculations,the OER performance of 27 types of C_(2)N-supported single transition metal atoms(TM@C_(2)N)is systematically investigated without and with considering the dynamic adsorption of possible intermediates.Without considering dynamic adsorption,only Rh@C_(2)N and Ni@C_(2)N are screened out as good catalysts.However,by further considering the dynamic adsorption configurations of possible intermediates,more promising TM@C_(2)N SACs including Fe(Co,Ni,Ru,Rh,Ir)@C_(2)N toward the OER are screened out.The presence of the intermediates(*HO,*O)on SACs could shift their d band center toward lower energy level,which makes the interaction between the adsorbate and SACs moderate and thus enhances their OER performance.The present work is instructive for further screening and designing of efficient single-atom catalysts for the oxygen evolution reaction.展开更多
In order to solve the problem of poor traveling stability and excessive pesticide application during plant protection operations in hilly orchards,a novel crawler-type multi-channel air-assisted sprayer that is partic...In order to solve the problem of poor traveling stability and excessive pesticide application during plant protection operations in hilly orchards,a novel crawler-type multi-channel air-assisted sprayer that is particularly appropriate for hilly orchards was designed in this study.Considering anti-rolling requirements and the orchard environment in hilly areas,this study selected limits for uphill and downhill rolling angles as well as the transverse rolling angle as the evaluation indexes for determining both the layout and parameter settings of the sprayer.According to freely submerged jets and the requirements in plant protection operation,a multi-channel air-assisted system was developed.The test results showed that the anti-rolling performance and the designed air-assisted system were adequate.At 2 m from the longitudinal center plane of the sprayer,the airflow exhibited wavy distribution patterns under different parameter combinations since the four streams of the airflow were not thoroughly intersected and mixed.At 3 m from the longitudinal center plane of the sprayer,the jet was ejected at great velocity but underwent rapid attenuation;the airflow velocity in most areas barely satisfied the requirements for plant protection operation.In addition,different air outlet layout schemes led to significant differences in the spatial distribution of the airflow field.Compared with a traditional air-assisted sprayer,using the developed multi-channel air-assisted sprayer enhanced the droplet coverage uniformity by 19.4%,and the mean droplet deposition in the front,middle,and rear of the canopy was enhanced by 32.9%,50.3%,and 78.1%,respectively,while reducing ground deposition and air drift by 26.8%.展开更多
基金This work is supported by the National Key Research and Development Program(No.2018YFA0208600)the National Natural Science Foundation of Chi-na(No.U19A2015,No.22102167)+2 种基金CAS Project for Young Scientists in Basic Research(YSBR-051)Wenhua Zhang is supported by USTC Tang Scholarship and State Scholarship Fund(202206345005)The calculations were performed at the Super-computing Center of University of Science and Technology of China(USTCSCC).
文摘The dynamic adsorption of possible intermediates on single-atom catalysts(SACs)under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction(OER),and therefore the performance of the dynamic adsorption should be fully considered in the theoretical screening of potential SACs.Based on density functional theory calculations,the OER performance of 27 types of C_(2)N-supported single transition metal atoms(TM@C_(2)N)is systematically investigated without and with considering the dynamic adsorption of possible intermediates.Without considering dynamic adsorption,only Rh@C_(2)N and Ni@C_(2)N are screened out as good catalysts.However,by further considering the dynamic adsorption configurations of possible intermediates,more promising TM@C_(2)N SACs including Fe(Co,Ni,Ru,Rh,Ir)@C_(2)N toward the OER are screened out.The presence of the intermediates(*HO,*O)on SACs could shift their d band center toward lower energy level,which makes the interaction between the adsorbate and SACs moderate and thus enhances their OER performance.The present work is instructive for further screening and designing of efficient single-atom catalysts for the oxygen evolution reaction.
基金This project was supported by the National Natural Science Foundation of China(Grant No.51805271)Jiangsu Agricultural Science and Technology Innovation Fund(CX181007)and Fundamental Research Funds for the Central Universities(KYYJ201805).
文摘In order to solve the problem of poor traveling stability and excessive pesticide application during plant protection operations in hilly orchards,a novel crawler-type multi-channel air-assisted sprayer that is particularly appropriate for hilly orchards was designed in this study.Considering anti-rolling requirements and the orchard environment in hilly areas,this study selected limits for uphill and downhill rolling angles as well as the transverse rolling angle as the evaluation indexes for determining both the layout and parameter settings of the sprayer.According to freely submerged jets and the requirements in plant protection operation,a multi-channel air-assisted system was developed.The test results showed that the anti-rolling performance and the designed air-assisted system were adequate.At 2 m from the longitudinal center plane of the sprayer,the airflow exhibited wavy distribution patterns under different parameter combinations since the four streams of the airflow were not thoroughly intersected and mixed.At 3 m from the longitudinal center plane of the sprayer,the jet was ejected at great velocity but underwent rapid attenuation;the airflow velocity in most areas barely satisfied the requirements for plant protection operation.In addition,different air outlet layout schemes led to significant differences in the spatial distribution of the airflow field.Compared with a traditional air-assisted sprayer,using the developed multi-channel air-assisted sprayer enhanced the droplet coverage uniformity by 19.4%,and the mean droplet deposition in the front,middle,and rear of the canopy was enhanced by 32.9%,50.3%,and 78.1%,respectively,while reducing ground deposition and air drift by 26.8%.