Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the...Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the input energy is"wasted"at the anode due to the high overpotential requirement and the recovery of low-value oxygen.To make efficient use of the electricity during electrolysis,coupling CO_(2)RR with anodic alternatives that have low energy demands and/or profitable returns with high-value products is then promising.Herein,we review the latest advances in paired systems for simultaneous CO_(2) reduction and anode valorization.We start with the cases integrating CO_(2)RR with concurrent alternative oxidation,such as inorganic oxidation using chloride,sulfide,ammonia and urea,and organic oxidation using alcohols,aldehydes and primary amines.The paired systems that couple CO_(2)RR with on-site oxidative upgrading of CO_(2)-reduced chemicals are also introduced.The coupling mechanism,electrochemical performance and economic viability of these co-electrolysis systems are discussed.Thereby,we then point out the mismatch issues between the cathodic and anodic reactions regrading catalyst ability,electrolyte solution and reactant supply that will challenge the applications of these paired electrolysis systems.Opportunities to address these issues are further proposed,providing some guidance for future research.展开更多
The additive strategy has emerged as an effective approach to improving the performance of perovskite solar cells(PSCs).Herein,a small acceptor-donor-acceptor type molecule indaceno[1,2-b:5,6-b’]dithiophene chloride(...The additive strategy has emerged as an effective approach to improving the performance of perovskite solar cells(PSCs).Herein,a small acceptor-donor-acceptor type molecule indaceno[1,2-b:5,6-b’]dithiophene chloride(IDT-Cl)is designed and synthesized to advance both the efficiency and stability of FA_(0.85)MA_(0.15)PbI_(3)PSCs.Within the IDT-Cl molecule,the S-group with high electron density promotes chemical bonding with the lead cations in the perovskite,resulting in enlarged grain size and smoother surface topography of the perovskite absorber.In addition,the undercoordinated lead ions in the perovskite layer may be passivated by the carbonyl group in the 5-chloroindolin-2-one unit,thereby reducing the number of nonradiative recombination centers.Meanwhile,the IDT-Cl adjusts the energy level mismatch between the perovskite and two adjacent carrier transport layers,leading to easy charge collection.By the multifunctional effect of the IDT-Cl molecule,the modified device yields a high power conversion efficiency(PCE)of 24.46%,8.8%higher than that of the control PSC(22.48%).More importantly,the hydrophobic alkyl side-chain of the IDT-Cl molecule further ensures enhanced humidity stability of the perovskite film and environmental,thermal,and light stabilities of the PSC devices.展开更多
基金financially supported by the National Natural Science Foundation of China(22002084,22072081)the China Postdoctoral Science Foundation(2020M683420)+1 种基金the Fundamental Research Funds for the Central Universities(GK202103111)the 111 Project(B21005)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)holds great promise in green energy conversion and storage.However,for current CO_(2) electrolyzers that rely on the oxygen evolution reaction,a large portion of the input energy is"wasted"at the anode due to the high overpotential requirement and the recovery of low-value oxygen.To make efficient use of the electricity during electrolysis,coupling CO_(2)RR with anodic alternatives that have low energy demands and/or profitable returns with high-value products is then promising.Herein,we review the latest advances in paired systems for simultaneous CO_(2) reduction and anode valorization.We start with the cases integrating CO_(2)RR with concurrent alternative oxidation,such as inorganic oxidation using chloride,sulfide,ammonia and urea,and organic oxidation using alcohols,aldehydes and primary amines.The paired systems that couple CO_(2)RR with on-site oxidative upgrading of CO_(2)-reduced chemicals are also introduced.The coupling mechanism,electrochemical performance and economic viability of these co-electrolysis systems are discussed.Thereby,we then point out the mismatch issues between the cathodic and anodic reactions regrading catalyst ability,electrolyte solution and reactant supply that will challenge the applications of these paired electrolysis systems.Opportunities to address these issues are further proposed,providing some guidance for future research.
基金supported by the National Natural Science Foundation of China(62174103,62274104)the Fundamental Research Funds for the Central Universities(GK202103052)+2 种基金the Changjiang Scholar and the Innovative Research Team(IRT_14R33)the 111 Project(B21005)the Chinese National 1000-Talent-Plan Program(111001034)。
文摘The additive strategy has emerged as an effective approach to improving the performance of perovskite solar cells(PSCs).Herein,a small acceptor-donor-acceptor type molecule indaceno[1,2-b:5,6-b’]dithiophene chloride(IDT-Cl)is designed and synthesized to advance both the efficiency and stability of FA_(0.85)MA_(0.15)PbI_(3)PSCs.Within the IDT-Cl molecule,the S-group with high electron density promotes chemical bonding with the lead cations in the perovskite,resulting in enlarged grain size and smoother surface topography of the perovskite absorber.In addition,the undercoordinated lead ions in the perovskite layer may be passivated by the carbonyl group in the 5-chloroindolin-2-one unit,thereby reducing the number of nonradiative recombination centers.Meanwhile,the IDT-Cl adjusts the energy level mismatch between the perovskite and two adjacent carrier transport layers,leading to easy charge collection.By the multifunctional effect of the IDT-Cl molecule,the modified device yields a high power conversion efficiency(PCE)of 24.46%,8.8%higher than that of the control PSC(22.48%).More importantly,the hydrophobic alkyl side-chain of the IDT-Cl molecule further ensures enhanced humidity stability of the perovskite film and environmental,thermal,and light stabilities of the PSC devices.