Although Ti3 C2 MXene sheets have attracted extensive attention in lithium-ion storage techniques,their restacking makes against and even hinders the Li ions diffusion within them,thereby decreasing the capacity as we...Although Ti3 C2 MXene sheets have attracted extensive attention in lithium-ion storage techniques,their restacking makes against and even hinders the Li ions diffusion within them,thereby decreasing the capacity as well as rate performance of conventional MXene anode.Here,for the first time,we roll up the Ti3 C2 Tx sheets into scrolls with unclosed topological structure and the interlayer galleries to alleviate the restacking problem.Thus,Ti3 C2 Tx scrolls as anode materials in lithium-ion batteries(LIBs)have higher capacity and better rate performance than Ti3 C2 Tx sheets.On the bases of these,high-capacity silicon nanoparticles are added during the rolling process to in-situ produce Ti3 C2 Tx/Si composite scrolls.The addition of 10%silicon nanoparticles shows the best overall improvement among capacity,rate capability and cyclic stability for Ti3 C2 Tx scrolls.展开更多
Hydrogen evolution by electrocatalysis clean energy. However, it is challenging is an attractive method of supplying to find cheap and efficient alternatives to rare and expensive platinum based catalysts. Pt provides...Hydrogen evolution by electrocatalysis clean energy. However, it is challenging is an attractive method of supplying to find cheap and efficient alternatives to rare and expensive platinum based catalysts. Pt provides the best hydrogen evolution performance, because it optimally balances the free energies of adsorption and desorption. Appropriate control of these quantities is essential for producing an efficient electrocatalyst. We demonstrate, based on first principles calculations, a stepwise designed Rh-Au-Si ternary catalyst, in which adsorption (the Volmer reaction) and desorption (the Heyrovsky reaction) take place on Rh and Si surfaces, respectively. The intermediate Au surface plays a vital role by promoting hydrogen diffusion from the Rh to the Si surface. Theoretical predictions have been explored extensively and verified by experimental observations. The optimized catalyst (Rh-Au-SiNW-2) has a com- position of 2.2:28.5:69.3 (Rh:Au:Si mass ratio) and exhibits a Tafel slope of 24.0 mV.dec-L Its electrocatalytic activity surpasses that of a commercial 40 wt.% Pt/C catalyst at overpotentials above 0.19 V by exhibiting a current density of greater than 108 mA-cm-2. At 0.3 V overpotential, the turnover frequency of Rh-Au-SiNW-2 is 10.8 times greater than that of 40 wt.% Pt/C. These properties may open new directions in the stepwise design of highly efficient catalysts for the hydrogen evolution reaction (HER).展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21573265,21673263,and 21805291)One-Three-Five Strategic Planning of Chinese Academy of Sciences and the DNL Cooperation Fund,CAS(DNL180307)。
文摘Although Ti3 C2 MXene sheets have attracted extensive attention in lithium-ion storage techniques,their restacking makes against and even hinders the Li ions diffusion within them,thereby decreasing the capacity as well as rate performance of conventional MXene anode.Here,for the first time,we roll up the Ti3 C2 Tx sheets into scrolls with unclosed topological structure and the interlayer galleries to alleviate the restacking problem.Thus,Ti3 C2 Tx scrolls as anode materials in lithium-ion batteries(LIBs)have higher capacity and better rate performance than Ti3 C2 Tx sheets.On the bases of these,high-capacity silicon nanoparticles are added during the rolling process to in-situ produce Ti3 C2 Tx/Si composite scrolls.The addition of 10%silicon nanoparticles shows the best overall improvement among capacity,rate capability and cyclic stability for Ti3 C2 Tx scrolls.
文摘Hydrogen evolution by electrocatalysis clean energy. However, it is challenging is an attractive method of supplying to find cheap and efficient alternatives to rare and expensive platinum based catalysts. Pt provides the best hydrogen evolution performance, because it optimally balances the free energies of adsorption and desorption. Appropriate control of these quantities is essential for producing an efficient electrocatalyst. We demonstrate, based on first principles calculations, a stepwise designed Rh-Au-Si ternary catalyst, in which adsorption (the Volmer reaction) and desorption (the Heyrovsky reaction) take place on Rh and Si surfaces, respectively. The intermediate Au surface plays a vital role by promoting hydrogen diffusion from the Rh to the Si surface. Theoretical predictions have been explored extensively and verified by experimental observations. The optimized catalyst (Rh-Au-SiNW-2) has a com- position of 2.2:28.5:69.3 (Rh:Au:Si mass ratio) and exhibits a Tafel slope of 24.0 mV.dec-L Its electrocatalytic activity surpasses that of a commercial 40 wt.% Pt/C catalyst at overpotentials above 0.19 V by exhibiting a current density of greater than 108 mA-cm-2. At 0.3 V overpotential, the turnover frequency of Rh-Au-SiNW-2 is 10.8 times greater than that of 40 wt.% Pt/C. These properties may open new directions in the stepwise design of highly efficient catalysts for the hydrogen evolution reaction (HER).