Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive r...Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.展开更多
PM_(2.5)concentrations have dramatically reduced in key regions of China during the period 2013-2017,while O_(3)has increased.Hence there is an urgent demand to develop a synergetic regional PM_(2.5)and O_(3)control s...PM_(2.5)concentrations have dramatically reduced in key regions of China during the period 2013-2017,while O_(3)has increased.Hence there is an urgent demand to develop a synergetic regional PM_(2.5)and O_(3)control strategy.This study develops an emission-to-concentration response surface model and proposes a synergetic pathway for PM_(2.5)and O_(3)control in the Yangtze River Delta(YRD)based on the framework of the Air Benefit and Cost and Attainment Assessment System(ABaCAS).Results suggest that the regional emissions of NOx,SO_(2),NH3,VOCs(volatile organic compounds)and primary PM_(2.5)should be reduced by 18%,23%,14%,17%and 33%compared with 2017 to achieve 25%and 5% decreases of PM_(2.5)and O_(3)in 2025,and that the emission reduction ratios will need to be 50%,26%,28%,28% and 55%to attain the National Ambient Air Quality Standard.To effectively reduce the O_(3) pollution in the central and eastern YRD,VOCs controls need to be strengthened to reduce O_(3)by 5%,and then NOx reduction should be accelerated for air quality attainment.Meanwhile,control of primary PM_(2.5)emissions shall be prioritized to address the severe PM_(2.5)pollution in the northern YRD.For most cities in the YRD,the VOCs emission reduction ratio should be higher than that for NOx in Spring and Autumn.NOx control should be increased in summer rather than winter when a strong VOC-limited regime occurs.Besides,regarding the emission control of industrial processes,on-road vehicle and residential sources shall be prioritized and the joint control area should be enlarged to include Shandong,Jiangxi and Hubei Province for effective O_(3)control.展开更多
Despite millions of seafarers and passengers staying on ships each year, few studies have been conducted on the indoor air quality inside ship hulls. In this study, we investigated the levels and size distribution of ...Despite millions of seafarers and passengers staying on ships each year, few studies have been conducted on the indoor air quality inside ship hulls. In this study, we investigated the levels and size distribution of indoor particulate matter during two cruises of the research vessel “Xuelong” from Shanghai to Antarctica. The results showed that the particle size less than 2.5 μm(PM_(2.5)), and particle size less than 10 μm(PM_(10)) concentrations in different rooms of the ship widely varied. We observed high particulate matter(PM) levels in some of the rooms. The mass concentration distribution was dominated by 1–4 μm particles, which may have been caused by the hygroscopic growth of fine particles. The dominant factors influencing PM concentrations were indoor temperature, relative humidity, and human activity. We quantified contributions of these factors to the levels of indoor particles using a generalized additive model. In clean rooms, the levels of indoor particles were controlled by temperature and relative humidity, whereas in polluted rooms, the levels of indoor particles were mainly influenced by temperature and human activity, which implied that controlling temperature and human activity would efficiently reduce the levels of indoor particles.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government,Ministry of Science and ICT(MSIT)(NRF-2020M3D1A2102837)the Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(20214000000500,training program of CCUS for the green growth)。
文摘Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.
基金supported by the Key Projects of National Key Research and Development Program of the Ministry of Science and Technology of China(No.2018YFC0213805)Shanghai Science and Technology Commission Scientific Research Project(No.19DZ1205006)+2 种基金the National Natural Science Foundation of China(Nos.92044302 and 21625701)the Samsung Advanced Institute of Technologysupported by the Tencent Foundation through the Explorer Prize。
文摘PM_(2.5)concentrations have dramatically reduced in key regions of China during the period 2013-2017,while O_(3)has increased.Hence there is an urgent demand to develop a synergetic regional PM_(2.5)and O_(3)control strategy.This study develops an emission-to-concentration response surface model and proposes a synergetic pathway for PM_(2.5)and O_(3)control in the Yangtze River Delta(YRD)based on the framework of the Air Benefit and Cost and Attainment Assessment System(ABaCAS).Results suggest that the regional emissions of NOx,SO_(2),NH3,VOCs(volatile organic compounds)and primary PM_(2.5)should be reduced by 18%,23%,14%,17%and 33%compared with 2017 to achieve 25%and 5% decreases of PM_(2.5)and O_(3)in 2025,and that the emission reduction ratios will need to be 50%,26%,28%,28% and 55%to attain the National Ambient Air Quality Standard.To effectively reduce the O_(3) pollution in the central and eastern YRD,VOCs controls need to be strengthened to reduce O_(3)by 5%,and then NOx reduction should be accelerated for air quality attainment.Meanwhile,control of primary PM_(2.5)emissions shall be prioritized to address the severe PM_(2.5)pollution in the northern YRD.For most cities in the YRD,the VOCs emission reduction ratio should be higher than that for NOx in Spring and Autumn.NOx control should be increased in summer rather than winter when a strong VOC-limited regime occurs.Besides,regarding the emission control of industrial processes,on-road vehicle and residential sources shall be prioritized and the joint control area should be enlarged to include Shandong,Jiangxi and Hubei Province for effective O_(3)control.
基金supported by the National Natural Science Foundation of China (Nos. 41941014, 41676173)the Ministry of Natural Resources of the People’s Republic of China (No. IRASCC_(2)020-2022-No.01-01-02E)supported by China Arctic and Antarctic Administration。
文摘Despite millions of seafarers and passengers staying on ships each year, few studies have been conducted on the indoor air quality inside ship hulls. In this study, we investigated the levels and size distribution of indoor particulate matter during two cruises of the research vessel “Xuelong” from Shanghai to Antarctica. The results showed that the particle size less than 2.5 μm(PM_(2.5)), and particle size less than 10 μm(PM_(10)) concentrations in different rooms of the ship widely varied. We observed high particulate matter(PM) levels in some of the rooms. The mass concentration distribution was dominated by 1–4 μm particles, which may have been caused by the hygroscopic growth of fine particles. The dominant factors influencing PM concentrations were indoor temperature, relative humidity, and human activity. We quantified contributions of these factors to the levels of indoor particles using a generalized additive model. In clean rooms, the levels of indoor particles were controlled by temperature and relative humidity, whereas in polluted rooms, the levels of indoor particles were mainly influenced by temperature and human activity, which implied that controlling temperature and human activity would efficiently reduce the levels of indoor particles.