The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped c...The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.展开更多
A one-dimensional modified integral equation for electromagnetic scattering from a metallic concentric disc-ring structure is derived by using Fourier expansion and separating the contribution of charge density from c...A one-dimensional modified integral equation for electromagnetic scattering from a metallic concentric disc-ring structure is derived by using Fourier expansion and separating the contribution of charge density from conventional EFIE. In the case of normal incidence, the derived equation is very simple and easy to be solved numerically regardless of the electric dimension of the structure. The comparison between the data of RCS of a disc by using this method and analytical method shows the effectiveness of this approach. Numerical results are also given for current distributions and the scattered fields for a disc-ring structure.展开更多
A rotating ring (Pt) disc (Pt) electrode was employed to investigate the oxidation process of sodium sulfide (Na 2S). It was reported that the oxidation intermediates and product of HS - were formed on the disc electr...A rotating ring (Pt) disc (Pt) electrode was employed to investigate the oxidation process of sodium sulfide (Na 2S). It was reported that the oxidation intermediates and product of HS - were formed on the disc electrode and then reduced on the ring electrode. The results indicate that at a rotation rate of 20 Hz, when the disc electrode potential was -0.15 V (vs SHE) and higher, more extensive oxidation process took place via a series of electrochemical steps to produce sulfur (S). The products of oxidation intermediates (S 2- x , S 2- 2) and sulfur (S) reduced either on the ring electrode with a set potential of -0.8 V (vs SHE), or on disc electrode with negative going potential sweep at about -0.5～ 0.55 V (vs SHE). The experimental results of voltammogram of ring disc electrode at sodium sulfide solution demonstrated that the first step was the oxidation of HS - and produce S 2- x , and then the S 2- x adsorbed integrated itself and formed sulfur (S).展开更多
基金Grant PID2020-115848RB-C21 "STORELEC" projectTED2021-129694B-C22 "DEFY-CO2" project funded by MCIN/AEI/10.13039/501100011033+3 种基金LMP253_ (2)1 project funded by Gobierno de AragónGrant IJC2019-041874-I funded by the MCIN/AEI/10.13039/501100011033CSIC for her JAE Intro ICU 2021-ICB-04 grantthe Y2020/EMT-6419 "CEOTRES" project funded by the Comunidad Autonoma de Madrid。
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR) to controllable chemicals is considered as a promising pathway to store intermittent renewable energy. Herein, a set of catalysts based on copper-nitrogendoped carbon xerogel(Cu-N-C) are successfully developed varying the copper amount and the nature of the copper precursor, for the efficient CO_(2)RR. The electrocatalytic performance of Cu-N-C materials is assessed by a rotating ring-disc electrode(RRDE), technique still rarely explored for CO_(2)RR. For comparison, products are also characterized by online gas chromatography in a H-cell. The as-synthesized Cu-NC catalysts are found to be active and highly CO selective at low overpotentials(from -0.6 to -0.8 V vs.RHE) in 0.1 M KHCO_(3), while H_(2) from the competitive water reduction appears at larger overpotentials(-0.9 V vs. RHE). The optimum copper acetate-derived catalyst containing Cu-N_(4) moieties exhibits a CO_(2)-to-CO turnover frequency of 997 h^(-1) at -0.9 V vs. RHE with a H_(2)/CO ratio of 1.8. These results demonstrate that RRDE configuration can be used as a feasible approach for identifying electrolysis products from CO_(2)RR.
文摘A one-dimensional modified integral equation for electromagnetic scattering from a metallic concentric disc-ring structure is derived by using Fourier expansion and separating the contribution of charge density from conventional EFIE. In the case of normal incidence, the derived equation is very simple and easy to be solved numerically regardless of the electric dimension of the structure. The comparison between the data of RCS of a disc by using this method and analytical method shows the effectiveness of this approach. Numerical results are also given for current distributions and the scattered fields for a disc-ring structure.
文摘A rotating ring (Pt) disc (Pt) electrode was employed to investigate the oxidation process of sodium sulfide (Na 2S). It was reported that the oxidation intermediates and product of HS - were formed on the disc electrode and then reduced on the ring electrode. The results indicate that at a rotation rate of 20 Hz, when the disc electrode potential was -0.15 V (vs SHE) and higher, more extensive oxidation process took place via a series of electrochemical steps to produce sulfur (S). The products of oxidation intermediates (S 2- x , S 2- 2) and sulfur (S) reduced either on the ring electrode with a set potential of -0.8 V (vs SHE), or on disc electrode with negative going potential sweep at about -0.5～ 0.55 V (vs SHE). The experimental results of voltammogram of ring disc electrode at sodium sulfide solution demonstrated that the first step was the oxidation of HS - and produce S 2- x , and then the S 2- x adsorbed integrated itself and formed sulfur (S).
