The substitution of TiO_(2)for SiO_(2)in Y_(2)O_(3)-Li_(2)O-Al_(2)O_(3)-SiO_(2)(YLAS)glass-ceramics significantly altered their crystallization behavior and properties.Introducing TiO_(2)reduced the glass transition t...The substitution of TiO_(2)for SiO_(2)in Y_(2)O_(3)-Li_(2)O-Al_(2)O_(3)-SiO_(2)(YLAS)glass-ceramics significantly altered their crystallization behavior and properties.Introducing TiO_(2)reduced the glass transition temperature while increasing the crystallization peak temperature and lowering activation energy,which facilitated crystallization.The crystal growth shifted from three-dimensional to two-dimensional,and the primary phases transitioned from Al_(9.83)Zr_(0.17)and Y_(2)Si_(2)O_(7)to Y_(4.67)(SiO_(4))_(3)O,though crystal morphology remained unchanged.Grain size increased with higher crystallization temperatures.Mechanically,Vickers hardness slightly decreased(from 796 to 784 Hv),while bending strength improved(from 141 to 146 MPa),suggesting that TiO_(2)enhanced toughness without compromising structural integrity.The strength of the glass can be further improved through two-step ion exchange,but excessive crystallization can lead to cracks on the glass surface due to excessive surface compressive stress,resulting in a decrease in bending strength.These findings provide critical insights for optimizing YLAS glass-ceramics for advanced applications.展开更多
The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative...The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system,but the catalyst layer in direct contact with the hydrated proton environment usually leads to H_(2)evolution dominating.Herein,we show that polydimethyldiallyl-ammonium-chloride-coated Ag(Ag@PDDA)electrode exhibits outstanding performance with a FE of 86%,a single-pass conversion of 72%,and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl)decorated Ag(Ag/QAPPT)and cetyltrimethylammonium bromide decorated Ag(Ag/CTAB).The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer,which not only suppresses the migration of H+during the electrolysis process and blocks the direct contact between H2O and Ag catalyst,but also promotes the generation from CO_(2)to*COOH in a pure-acid system.This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO_(2)electrolysis.展开更多
基金Funded by the China Building Material Federation Projects(Nos.20221JBGS06-19 and 2023JBGS02-01)。
文摘The substitution of TiO_(2)for SiO_(2)in Y_(2)O_(3)-Li_(2)O-Al_(2)O_(3)-SiO_(2)(YLAS)glass-ceramics significantly altered their crystallization behavior and properties.Introducing TiO_(2)reduced the glass transition temperature while increasing the crystallization peak temperature and lowering activation energy,which facilitated crystallization.The crystal growth shifted from three-dimensional to two-dimensional,and the primary phases transitioned from Al_(9.83)Zr_(0.17)and Y_(2)Si_(2)O_(7)to Y_(4.67)(SiO_(4))_(3)O,though crystal morphology remained unchanged.Grain size increased with higher crystallization temperatures.Mechanically,Vickers hardness slightly decreased(from 796 to 784 Hv),while bending strength improved(from 141 to 146 MPa),suggesting that TiO_(2)enhanced toughness without compromising structural integrity.The strength of the glass can be further improved through two-step ion exchange,but excessive crystallization can lead to cracks on the glass surface due to excessive surface compressive stress,resulting in a decrease in bending strength.These findings provide critical insights for optimizing YLAS glass-ceramics for advanced applications.
基金financial support of the National Natural Science Foundation of China(NSFC)(52394202,52021004,52301232,and 52476056)the Natural Science Foundation of Chongqing Province(2024NSCQ-MSX1109).
文摘The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system,but the catalyst layer in direct contact with the hydrated proton environment usually leads to H_(2)evolution dominating.Herein,we show that polydimethyldiallyl-ammonium-chloride-coated Ag(Ag@PDDA)electrode exhibits outstanding performance with a FE of 86%,a single-pass conversion of 72%,and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl)decorated Ag(Ag/QAPPT)and cetyltrimethylammonium bromide decorated Ag(Ag/CTAB).The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer,which not only suppresses the migration of H+during the electrolysis process and blocks the direct contact between H2O and Ag catalyst,but also promotes the generation from CO_(2)to*COOH in a pure-acid system.This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO_(2)electrolysis.
