Solar vapor generation(SVC)represents a promising technique for seawater desalination to alleviate the global water crisis and energy shortage.One of its main bottleneck problems is that the evaporation efficiency and...Solar vapor generation(SVC)represents a promising technique for seawater desalination to alleviate the global water crisis and energy shortage.One of its main bottleneck problems is that the evaporation efficiency and stability are limited by salt crystallization under high-salinity brines.Herein,we demonstrate that the 3D porous melamine-foam(MF)wrapped by a type of self-assembling composite materials based on reduced polyoxometalates(i.e.heteropoly blue,HPB),oleic acid(OA),and polypyrrole(PPy)(labeled with MF@HPB-PPy_(n)-OA)can serve as efficient and stable SVC material at high salinity.Structural characterizations of MF@HPB-PPy_(n)-OA indicate that both hydrophilic region of HPBs and hydrophobic region of OA co-exist on the surface of composite materials,optimizing the hydrophilic and hydrophobic interfaces of the SVC materials,and fully exerting its functionality for ultrahigh water-evaporation and anti-salt fouling.The optimal MF@HPB-PPy_(10)-OA operates continuously and stably for over 100 h in 10wt%brine.Furthermore,MF@HPB-PPy_(10)-OA accomplishes complete salt-water separation of 10wt%brine with 3.3kgm^(-2)h^(-1)under 1-sun irradiation,yielding salt harvesting efficiency of 96.5%,which belongs to the record high of high-salinity systems reported so far and is close to achieving zero liquid discharge.Moreover,the low cost of MF@HPB-PPy_(10)-OA(2.56$m^(-2))suggests its potential application in the practical SVC technique.展开更多
Hydrothermal reactions of Na2MoO2·2H2O and NH4VO3（or V2O5） with appropriate reducing agents such as organic amines, NH2OH·HCl and Mo（CO）6 gave rise to the formation of a series of capped Keggin derivativ...Hydrothermal reactions of Na2MoO2·2H2O and NH4VO3（or V2O5） with appropriate reducing agents such as organic amines, NH2OH·HCl and Mo（CO）6 gave rise to the formation of a series of capped Keggin derivatives, [N（CH3）4]2Na3（NH4）2[（V^VO4）Mo^VI8V^IV4O36（V^IVO）2]·-13H2O（1）, [NH4]7[（V^VO4）Mo^VI8V^IV4O36（V^IVO）2]·7H2O（2）, [HN（CH2CH2）3NH][（PO4）Mo^V3Mo^VI9O36（V^IVO）2]·-3[N（CH2CH2）3N]·（en）·4.5H2O（3） and [HNH2OH][NH4]2[（V^VO4）Mo^VI8V^IV4O36（V^IVO）4]·24H2O（4）. Single-crystal X-ray diffraction analysis revealed that the anions in 1-3 are two-capped Keggin derivatives with characteristic trans vanadium-oxygen caps, whereas the heteropoly anion in 4 is a tetra-capped α-Keggin derivative with characteristic vanadium-oxygen caps on the equatorial plane.展开更多
The synergistic effect of H_3PMo_(12)O_(40) or H_3PW_(12)O_(40) polyoxometalate solution(POM) and TiO_2 to catalyze formic acid oxidation was investigated. Under UV irradiation, hole and electron were photogenerated b...The synergistic effect of H_3PMo_(12)O_(40) or H_3PW_(12)O_(40) polyoxometalate solution(POM) and TiO_2 to catalyze formic acid oxidation was investigated. Under UV irradiation, hole and electron were photogenerated by TiO_2. Formic acid was oxided by the photogenerated hole and photogenerated electron was transferred to reduce polyoxometalate. With this design, formic acid can be converted into electricity in the fuel cell and hydrogen can be generated in the electrolysis cell without noble metal catalyst. Unlike other noble metal catalysts applied in the fuel cells and electrolysis cell, POM and TiO_2 are stable and low cost. The maximum output power density of liquid formic acid fuel cell after 12 h UV irradiation is 5.21 mW/cm^2 for phosphmolybdic acid and 22.81 m W/cm^2 for phosphotungstic acid respectively. The applied potential for the hydrogen evolution is as low as 0.8 V for phosphmolybdic acid and 0.6 V for phosphotungstic acid.展开更多
在锂离子电池(LIBs)和钠离子电池(SIBs)中,设计同时适用的负极材料,使其具有高倍率性能和超长循环寿命是亟需解决的工作。本文采用静电纺丝技术和硫化工程技术成功制备了一种均匀分布在N,S-掺杂炭纳米纤维上的MoO_(2)/MoS_(2)异质结构(M...在锂离子电池(LIBs)和钠离子电池(SIBs)中,设计同时适用的负极材料,使其具有高倍率性能和超长循环寿命是亟需解决的工作。本文采用静电纺丝技术和硫化工程技术成功制备了一种均匀分布在N,S-掺杂炭纳米纤维上的MoO_(2)/MoS_(2)异质结构(MoO_(2)/MoS_(2)@NSC)。其中一维炭骨架作为导电框架可缩短Li^(+)/Na^(+)的扩散途径;炭纳米纤维中N/S杂原子的掺杂引入了丰富的活性位点,显著增强了离子扩散动力学。此外,在MoO_(2)相中通过原位形成的MoS_(2)纳米片强化了异质界面,MoO_(2)和MoS_(2)之间异质界面的构建使得Li^(+)/Na^(+)的快速传输成为实现高效储能的关键。因此,作为LIBs负极材料时,MoO_(2)/MoS_(2)@NSC电极在5.0 A g^(−1)的电流密度下循环2000圈后,仍具有640 mAh g^(−1)的优异放电比容量,每圈的容量衰减率仅为0.002%;在10.0 A g^(−1)的高电流密度下可达到614 mAh g^(−1)的放电比容量。对于SIBs,在2.0 A g^(−1)的电流密度下循环2000圈后其可逆容量仍能达到242 mAh g^(−1)。本工作采用一种新颖的界面调控策略来合理地设计负极材料,从而提高Li^(+)/Na^(+)储存动力学,实现超长寿命的循环性能。展开更多
基金financially supported by the National Key Basic Research Program of China(grant no.2020YFA0406101)National Natural Science Foundation of China(grant nos.22171041,22071020,21901035,22271043)+1 种基金Natural Science Foundation of Jilin Province Science and Technology Department(grant nos.20230508094RC,20220101045JC)the Fundamental Research Funds for the Central Universities(grant no.2412021QD008)
文摘Solar vapor generation(SVC)represents a promising technique for seawater desalination to alleviate the global water crisis and energy shortage.One of its main bottleneck problems is that the evaporation efficiency and stability are limited by salt crystallization under high-salinity brines.Herein,we demonstrate that the 3D porous melamine-foam(MF)wrapped by a type of self-assembling composite materials based on reduced polyoxometalates(i.e.heteropoly blue,HPB),oleic acid(OA),and polypyrrole(PPy)(labeled with MF@HPB-PPy_(n)-OA)can serve as efficient and stable SVC material at high salinity.Structural characterizations of MF@HPB-PPy_(n)-OA indicate that both hydrophilic region of HPBs and hydrophobic region of OA co-exist on the surface of composite materials,optimizing the hydrophilic and hydrophobic interfaces of the SVC materials,and fully exerting its functionality for ultrahigh water-evaporation and anti-salt fouling.The optimal MF@HPB-PPy_(10)-OA operates continuously and stably for over 100 h in 10wt%brine.Furthermore,MF@HPB-PPy_(10)-OA accomplishes complete salt-water separation of 10wt%brine with 3.3kgm^(-2)h^(-1)under 1-sun irradiation,yielding salt harvesting efficiency of 96.5%,which belongs to the record high of high-salinity systems reported so far and is close to achieving zero liquid discharge.Moreover,the low cost of MF@HPB-PPy_(10)-OA(2.56$m^(-2))suggests its potential application in the practical SVC technique.
基金Supported by the 973 key program of the MOST(2010CB933501,2012CB821705)the Chinese Academy of Sciences(KJCX2-YW-319,KJCX2-EW-H01)+1 种基金the National Natural Science Foundation of China(21373221,21221001,91022008,91122027,51172232)the Natural Science Foundation of Fujian Province(2011HZ0001-1,2012J06006,2006L2005)
文摘Hydrothermal reactions of Na2MoO2·2H2O and NH4VO3（or V2O5） with appropriate reducing agents such as organic amines, NH2OH·HCl and Mo（CO）6 gave rise to the formation of a series of capped Keggin derivatives, [N（CH3）4]2Na3（NH4）2[（V^VO4）Mo^VI8V^IV4O36（V^IVO）2]·-13H2O（1）, [NH4]7[（V^VO4）Mo^VI8V^IV4O36（V^IVO）2]·7H2O（2）, [HN（CH2CH2）3NH][（PO4）Mo^V3Mo^VI9O36（V^IVO）2]·-3[N（CH2CH2）3N]·（en）·4.5H2O（3） and [HNH2OH][NH4]2[（V^VO4）Mo^VI8V^IV4O36（V^IVO）4]·24H2O（4）. Single-crystal X-ray diffraction analysis revealed that the anions in 1-3 are two-capped Keggin derivatives with characteristic trans vanadium-oxygen caps, whereas the heteropoly anion in 4 is a tetra-capped α-Keggin derivative with characteristic vanadium-oxygen caps on the equatorial plane.
文摘The synergistic effect of H_3PMo_(12)O_(40) or H_3PW_(12)O_(40) polyoxometalate solution(POM) and TiO_2 to catalyze formic acid oxidation was investigated. Under UV irradiation, hole and electron were photogenerated by TiO_2. Formic acid was oxided by the photogenerated hole and photogenerated electron was transferred to reduce polyoxometalate. With this design, formic acid can be converted into electricity in the fuel cell and hydrogen can be generated in the electrolysis cell without noble metal catalyst. Unlike other noble metal catalysts applied in the fuel cells and electrolysis cell, POM and TiO_2 are stable and low cost. The maximum output power density of liquid formic acid fuel cell after 12 h UV irradiation is 5.21 mW/cm^2 for phosphmolybdic acid and 22.81 m W/cm^2 for phosphotungstic acid respectively. The applied potential for the hydrogen evolution is as low as 0.8 V for phosphmolybdic acid and 0.6 V for phosphotungstic acid.
文摘在锂离子电池(LIBs)和钠离子电池(SIBs)中,设计同时适用的负极材料,使其具有高倍率性能和超长循环寿命是亟需解决的工作。本文采用静电纺丝技术和硫化工程技术成功制备了一种均匀分布在N,S-掺杂炭纳米纤维上的MoO_(2)/MoS_(2)异质结构(MoO_(2)/MoS_(2)@NSC)。其中一维炭骨架作为导电框架可缩短Li^(+)/Na^(+)的扩散途径;炭纳米纤维中N/S杂原子的掺杂引入了丰富的活性位点,显著增强了离子扩散动力学。此外,在MoO_(2)相中通过原位形成的MoS_(2)纳米片强化了异质界面,MoO_(2)和MoS_(2)之间异质界面的构建使得Li^(+)/Na^(+)的快速传输成为实现高效储能的关键。因此,作为LIBs负极材料时,MoO_(2)/MoS_(2)@NSC电极在5.0 A g^(−1)的电流密度下循环2000圈后,仍具有640 mAh g^(−1)的优异放电比容量,每圈的容量衰减率仅为0.002%;在10.0 A g^(−1)的高电流密度下可达到614 mAh g^(−1)的放电比容量。对于SIBs,在2.0 A g^(−1)的电流密度下循环2000圈后其可逆容量仍能达到242 mAh g^(−1)。本工作采用一种新颖的界面调控策略来合理地设计负极材料,从而提高Li^(+)/Na^(+)储存动力学,实现超长寿命的循环性能。
