The electrooxidation of Mn(Ⅱ) on Pb Sb As alloy electrode in sulfuric acid has been investigated.In order to make the two steps of indirect electrosynthesis of benzaldehyde carried out in the same sulfuric acid conce...The electrooxidation of Mn(Ⅱ) on Pb Sb As alloy electrode in sulfuric acid has been investigated.In order to make the two steps of indirect electrosynthesis of benzaldehyde carried out in the same sulfuric acid concentration and also obtain high current efficiency of Mn(Ⅱ) to Mn(Ⅲ) and high yield of Mn(Ⅲ) oxidizing toluene to benzaldehyde in the mean time,the electrooxidation of Mn(Ⅱ) in 60% H 2SO 4 has been studied.Experimental results show that high current efficiency of Mn(Ⅲ) (about 75%) is obtained in 60%H 2SO 4 at 60℃.The reason affecting the current efficiency of Mn(Ⅲ) is discussed,and it is the coordination of sulfuric acid concentration and electrolytic temperature.The law is found that it is suitable for electrolysis at low temperature when sulfuric acid concentration is low and at high temperature when sulfuric acid concentration is high.展开更多
Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effe...Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effect leads to severe capacity fading and low coulombic efficiency.Here,graphitic carbon nitride(g-C3N4) is designed and prepared via a feasible and simple method from trithiocyanuric acid (TTCA) to anchor the polysulfides and suppress the shuttle effect.The obtained g-C3N4 exhibits strong chemical interaction with polysulfides due to its high N-doping of 56.87 at%,which is beneficial to improve the cycling stability of Li-S batteries.Moreover,the novel porous framework and high specific surface area of g-C3N4 also provide fast ion transport and broad reaction interface of sulfur cathode,facilitating high capacity output and superior rate performance of Li-S batteries.As a result,Li-S batteries assembled with g-C3N4 can achieve high discharge capacity of 1200 mAh/g at 0.2 C and over 800 mAh/g is remained after 100 cycles with a coulombic efficiency more than 99.5%.When the C-rate rises to 5 C,the reversible capacity of Li-S batteries can still maintain at 607mAh/g.展开更多
The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caus...The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.展开更多
文摘The electrooxidation of Mn(Ⅱ) on Pb Sb As alloy electrode in sulfuric acid has been investigated.In order to make the two steps of indirect electrosynthesis of benzaldehyde carried out in the same sulfuric acid concentration and also obtain high current efficiency of Mn(Ⅱ) to Mn(Ⅲ) and high yield of Mn(Ⅲ) oxidizing toluene to benzaldehyde in the mean time,the electrooxidation of Mn(Ⅱ) in 60% H 2SO 4 has been studied.Experimental results show that high current efficiency of Mn(Ⅲ) (about 75%) is obtained in 60%H 2SO 4 at 60℃.The reason affecting the current efficiency of Mn(Ⅲ) is discussed,and it is the coordination of sulfuric acid concentration and electrolytic temperature.The law is found that it is suitable for electrolysis at low temperature when sulfuric acid concentration is low and at high temperature when sulfuric acid concentration is high.
基金the financial support from the National Natural Science Foundation of China(Nos.51673199 and 51677176)Youth Innovation Promotion Association of CAS(2015148)+1 种基金Innovation Foundation of DICP(ZZBS201615,ZZBS201708)Dalian Science and Technology Star Program(2016RQ026)。
文摘Lithium-sulfur (Li-S) batteries have great potential as an electrochemical energy storage system because of the high theoretical energy density and acceptable cost of financial and environment.However,the shuttle effect leads to severe capacity fading and low coulombic efficiency.Here,graphitic carbon nitride(g-C3N4) is designed and prepared via a feasible and simple method from trithiocyanuric acid (TTCA) to anchor the polysulfides and suppress the shuttle effect.The obtained g-C3N4 exhibits strong chemical interaction with polysulfides due to its high N-doping of 56.87 at%,which is beneficial to improve the cycling stability of Li-S batteries.Moreover,the novel porous framework and high specific surface area of g-C3N4 also provide fast ion transport and broad reaction interface of sulfur cathode,facilitating high capacity output and superior rate performance of Li-S batteries.As a result,Li-S batteries assembled with g-C3N4 can achieve high discharge capacity of 1200 mAh/g at 0.2 C and over 800 mAh/g is remained after 100 cycles with a coulombic efficiency more than 99.5%.When the C-rate rises to 5 C,the reversible capacity of Li-S batteries can still maintain at 607mAh/g.
基金supported by the National Natural Science Foundation of China(21875155,51675275,21703185 and 21473119)Q.B.Z.acknowledges the Leading Project Foundation of Science Department of Fujian Province(2018H0034)Shenzhen Science and Technology Planning Project(JCYJ20170818153427106).
文摘The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.
