m-Benzoquinones are often regarded as unstable materials in the form of radicals.Herein,an air-stable small molecular m-benzoquinone[4,6-diamino-1,3-benzoquinone(4,6DA1,3BQ)]without bulky groups or large conjugated sy...m-Benzoquinones are often regarded as unstable materials in the form of radicals.Herein,an air-stable small molecular m-benzoquinone[4,6-diamino-1,3-benzoquinone(4,6DA1,3BQ)]without bulky groups or large conjugated systems is reported,and its chemical structure and state are profoundly elucidated by a series of substantial investigations that indicate their presence as zwitterions rather than as diradicals.展开更多
The thermal decomposition of Ag NO_(3)is known to produce metallic Ag,but single-atomic dispersion is hard to achieve instead of the aggregation state of nanoparticles.Herein,we develop an efficient approach to therma...The thermal decomposition of Ag NO_(3)is known to produce metallic Ag,but single-atomic dispersion is hard to achieve instead of the aggregation state of nanoparticles.Herein,we develop an efficient approach to thermally generate and stabilize single Ag atoms via the coordination effect.Two desired Co-Ag phosphonates[Ag_(2)^(Ⅰ)Co_(2)^(Ⅲ)(notp H_(3))_2(NO_(3))]X[X=NO_(3)^(-)(1)or Cl O_(4)^(-)(2)]were synthesized by solid-phase grinding method or solution crystallization.Both crystal structures reveal slightly different packing arrangements of various lattice anions and identical one-dimensional(1-D)coordination chains,formed in each case by the coordination of Ag(Ⅰ)to the metalloligand Co(notp H_(3))and NO_(3)^(-) anion.The number of Ag(Ⅰ)ions connected to each NO_(3)^(-) anion reduces from 5 in bulk Ag NO_(3) to 2 in compounds 1 and 2,leading to the Ag NO_(3)component stepwise decomposition at a lower temperature(<300℃).During the thermal decomposition,the changes of supermolecular structures and Ag oxidation states were monitored by PXRD,IR and XAFS measurements.The most interesting finding is that 1 and 2 can retain chain structures and harvest Ag(0)atoms in the chain by controlling decomposition temperatures(220℃for 1 and 254℃for 2).展开更多
基金supported by the National Natural Science Foundation of China(nos.51773071 and 52173163)the National 1000-Talents Program,the Innovation Fund of WNLO,the Fundamental Research Funds for the Central Universities(HUST:nos.2018KFYXKJC018 and 2019kfyRCPY099)+1 种基金the Open Fund of the State Key Laboratory of Integrated Optoelectronics(no.IOSKL2020KF02)the China Postdoctoral Science Foundation(nos.2020M672323 and 2021TQ0115).
文摘m-Benzoquinones are often regarded as unstable materials in the form of radicals.Herein,an air-stable small molecular m-benzoquinone[4,6-diamino-1,3-benzoquinone(4,6DA1,3BQ)]without bulky groups or large conjugated systems is reported,and its chemical structure and state are profoundly elucidated by a series of substantial investigations that indicate their presence as zwitterions rather than as diradicals.
基金the National Natural Science Foundation of China(Nos.21671098,21731003)the Fundamental Research Funds for the Central Universities(Nos.14380151,14380206)is acknowledged。
文摘The thermal decomposition of Ag NO_(3)is known to produce metallic Ag,but single-atomic dispersion is hard to achieve instead of the aggregation state of nanoparticles.Herein,we develop an efficient approach to thermally generate and stabilize single Ag atoms via the coordination effect.Two desired Co-Ag phosphonates[Ag_(2)^(Ⅰ)Co_(2)^(Ⅲ)(notp H_(3))_2(NO_(3))]X[X=NO_(3)^(-)(1)or Cl O_(4)^(-)(2)]were synthesized by solid-phase grinding method or solution crystallization.Both crystal structures reveal slightly different packing arrangements of various lattice anions and identical one-dimensional(1-D)coordination chains,formed in each case by the coordination of Ag(Ⅰ)to the metalloligand Co(notp H_(3))and NO_(3)^(-) anion.The number of Ag(Ⅰ)ions connected to each NO_(3)^(-) anion reduces from 5 in bulk Ag NO_(3) to 2 in compounds 1 and 2,leading to the Ag NO_(3)component stepwise decomposition at a lower temperature(<300℃).During the thermal decomposition,the changes of supermolecular structures and Ag oxidation states were monitored by PXRD,IR and XAFS measurements.The most interesting finding is that 1 and 2 can retain chain structures and harvest Ag(0)atoms in the chain by controlling decomposition temperatures(220℃for 1 and 254℃for 2).