In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method...In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method involving high-pressure processing,stirring,and immiscible solutions,sub-100 nm MXene flake thickness is achieved within the MXene film on the Si-wafer.Functionalization control is achieved by defunctionalizing MXene at 650℃ under vacuum and H2 gas in a CVD furnace,followed by refunctionalization with iodine and bromine vaporization from a bubbler attached to the CVD.Notably,the introduction of iodine,which has a larger atomic size,lower electronegativity,reduce shielding effect,and lower hydrophilicity(contact angle:99°),profoundly affecting MXene.It improves the surface area(36.2 cm^(2) g^(-1)),oxidation stability in aqueous/ambient environments(21 days/80 days),and film conductivity(749 S m^(-1)).Additionally,it significantly enhances the gas-sensing performance,including the sensitivity(0.1119Ωppm^(-1)),response(0.2% and 23%to 50 ppb and 200 ppm NO_(2)),and response/recovery times(90/100 s).The reduced shielding effect of the–I-terminals and the metallic characteristics of MXene enhance the selectivity of I-MXene toward NO2.This approach paves the way for the development of stable and high-performance gas-sensing two-dimensional materials with promising prospects for future studies.展开更多
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT)(No. 2021R1I1A1A0105621313, No. 2022R1F1A1074441, No. 2022K1A3A1A20014496, and No. 2022R1F1A1074083)supported by the Ministry of Education Funding (No. RIS 2021-004)supported by the Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea (RS-2023-00284318).
文摘In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method involving high-pressure processing,stirring,and immiscible solutions,sub-100 nm MXene flake thickness is achieved within the MXene film on the Si-wafer.Functionalization control is achieved by defunctionalizing MXene at 650℃ under vacuum and H2 gas in a CVD furnace,followed by refunctionalization with iodine and bromine vaporization from a bubbler attached to the CVD.Notably,the introduction of iodine,which has a larger atomic size,lower electronegativity,reduce shielding effect,and lower hydrophilicity(contact angle:99°),profoundly affecting MXene.It improves the surface area(36.2 cm^(2) g^(-1)),oxidation stability in aqueous/ambient environments(21 days/80 days),and film conductivity(749 S m^(-1)).Additionally,it significantly enhances the gas-sensing performance,including the sensitivity(0.1119Ωppm^(-1)),response(0.2% and 23%to 50 ppb and 200 ppm NO_(2)),and response/recovery times(90/100 s).The reduced shielding effect of the–I-terminals and the metallic characteristics of MXene enhance the selectivity of I-MXene toward NO2.This approach paves the way for the development of stable and high-performance gas-sensing two-dimensional materials with promising prospects for future studies.
文摘基于Sentinel-5P卫星TROPOMI数据,利用随机森林方法反演2018~2020年淮河流域地面NO_(2)浓度,采用推算法获得淮河流域2018~2020年NO_(2)干沉降通量,并通过划分不同集水区(水域、农田、城区和植被覆盖区)估算大气NO_(2)干沉降对淮河流域水体氮素的贡献.结果显示,卫星反演地面NO_(2)浓度与地面站点实测资料一致性较高,相关系数(R)为0.94,平均绝对误差(MAE)为2.7,均方根误差(RSME)为4.1.淮河流域地面NO_(2)浓度和NO_(2)干沉降通量均有明显的季节变化,春夏秋冬4个季节地面NO_(2)平均浓度分别为13.7,12.2,17.6,23.1μg/m^(3);NO_(2)平均干沉降通量分别为1.25,1.13,1.61,2.13kg N/(hm^(2)·a).淮河流域地面NO_(2)浓度和干沉降通量均表现为南北部高,东西部低.农田区域NO_(2)干沉降对流域水体氮素的贡献最大,占比83.47%.2019年淮河流域大气NO_(2)干沉降总量为1.34×10^(5)t,对水体氮素的贡献为1.36×10^(4)t N;2020年大气NO_(2)干沉降总量为1.25×10^(5)t,对水体氮素的贡献为1.18×10^(4)t N.