The electric field-induced irreversible domain wall motion results in a ferroelectric(FE) hysteresis. In antiferroelectrics(AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which...The electric field-induced irreversible domain wall motion results in a ferroelectric(FE) hysteresis. In antiferroelectrics(AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis,the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr,Sn,Ti)O_(3) AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.展开更多
The inefficiency of ethanol oxidation reaction(EOR)presents a significant obstacle in harnessing renewable biofuels with high energy density into electricity.Despite efforts,most Pt-based catalysts still suffer from d...The inefficiency of ethanol oxidation reaction(EOR)presents a significant obstacle in harnessing renewable biofuels with high energy density into electricity.Despite efforts,most Pt-based catalysts still suffer from drawbacks such as poor activity and susceptibility to CO poisoning,particularly in acidic conditions.Herein,we employed a physical laser-assisted approach to synthetize a PtPd alloy with a 1:1 atomic ratio.This alloy demonstrates remarkable performance in acidic EOR,boasting a high mass activity of 1.86 A·mgPt^(−1)and competitive resistance to poisoning.Combining in situ synchrotron radiation infrared spectroscopy with theoretical calculations,we reveal that the synergic interaction between Pt and Pd enhances both the adsorption of OH*intermediate and the dehydrogenation ability of ethanol.This work will prove the feasibility of synthesizing bimetallic alloys by a physical laser-assisted strategy and promote the development of advanced alloy electrocatalysts.展开更多
Cubic silicon nitride(-Si_(3)N_(4))is superhard and one of the hardest materials after diamond and cubic boron nitride(cBN),but has higher thermal stability in an oxidizing environment than diamond,making it a competi...Cubic silicon nitride(-Si_(3)N_(4))is superhard and one of the hardest materials after diamond and cubic boron nitride(cBN),but has higher thermal stability in an oxidizing environment than diamond,making it a competitive candidate for technological applications in harsh conditions(e.g.,drill head and abrasives).Here,we report the high-pressure synthesis and characterization of the structural and mechanical properties of a γ-Si_(3)N_(4)/Hf_(3)N_(4) ceramic nanocomposite derived from single-phase amorphous silicon(Si)-hafnium(Hf)-nitrogen(N)precursor.The synthesis of the-Si_(3)N_(4)/Hf_(3)N_(4) nanocomposite is performed at~20 GPa and ca.1500 ℃ in a large volume multi anvil press.The structural evolution of the amorphous precursor and its crystallization to-Si_(3)N_(4)/Hf_(3)N_(4) nanocomposites under high pressures is assessed by the in situ synchrotron energy-dispersive X-ray diffraction(ED-XRD)measurements at~19.5 GPa in the temperature range of ca.1000-1900℃.The fracture toughness(K_(IC))of the two-phase nanocomposite amounts~6/6.9 MPa·m^(1/2) and is about 2 times that of single-phaseγ-Si_(3)N_(4),while its hardness of ca.30 GPa remains high.This work provides a reliable and feasible route for the synthesis of advanced hard and tough-Si_(3)N_(4)-based nanocomposites with excellent thermal stabililty.展开更多
基金supported by the National Natural Science Foundation of China (Nos.22235002, 21825102 and 12004032)the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No.DEAC02–06CH11357。
文摘The electric field-induced irreversible domain wall motion results in a ferroelectric(FE) hysteresis. In antiferroelectrics(AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis,the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr,Sn,Ti)O_(3) AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.
基金supported by the National Natural Science Foundation of China(Nos.12025505,12105287,22002147,22179125,U21A20317,and 22373001)the National Key Research and Development Program of China(No.2021YFA1600800)+3 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0450200)the Fundamental Research Funds for the Central Universities(No.KY2310000097)Xiaomi Young Talents Programsupported by the Supercomputing Center of the USTC.
文摘The inefficiency of ethanol oxidation reaction(EOR)presents a significant obstacle in harnessing renewable biofuels with high energy density into electricity.Despite efforts,most Pt-based catalysts still suffer from drawbacks such as poor activity and susceptibility to CO poisoning,particularly in acidic conditions.Herein,we employed a physical laser-assisted approach to synthetize a PtPd alloy with a 1:1 atomic ratio.This alloy demonstrates remarkable performance in acidic EOR,boasting a high mass activity of 1.86 A·mgPt^(−1)and competitive resistance to poisoning.Combining in situ synchrotron radiation infrared spectroscopy with theoretical calculations,we reveal that the synergic interaction between Pt and Pd enhances both the adsorption of OH*intermediate and the dehydrogenation ability of ethanol.This work will prove the feasibility of synthesizing bimetallic alloys by a physical laser-assisted strategy and promote the development of advanced alloy electrocatalysts.
基金Part of this research was carried out at PETRA III LVP at beamline P61B(beamtime I-20200434)and P02.1Shrikant Bhat and Robert Farla acknowedge the support from the Federal Ministry of Education and Research,Germany(BMBF,Nos.05K16WC2 and 05K13WC2)+2 种基金Wei Li and Leonore Wiehl also acknowledge the travel support from DESY.Zhaoju Yu thanks the National Natural Science Foundation of China(Nos.51872246 and 52061135102)for financial supportMarc Widenmeyer and Anke Weidenkaff are grateful for the financial support by the German Ministry of Education and Research(No.03SF0618B)Wei Li acknowledges the financial support from China Scholarship Council(No.201907040060).
文摘Cubic silicon nitride(-Si_(3)N_(4))is superhard and one of the hardest materials after diamond and cubic boron nitride(cBN),but has higher thermal stability in an oxidizing environment than diamond,making it a competitive candidate for technological applications in harsh conditions(e.g.,drill head and abrasives).Here,we report the high-pressure synthesis and characterization of the structural and mechanical properties of a γ-Si_(3)N_(4)/Hf_(3)N_(4) ceramic nanocomposite derived from single-phase amorphous silicon(Si)-hafnium(Hf)-nitrogen(N)precursor.The synthesis of the-Si_(3)N_(4)/Hf_(3)N_(4) nanocomposite is performed at~20 GPa and ca.1500 ℃ in a large volume multi anvil press.The structural evolution of the amorphous precursor and its crystallization to-Si_(3)N_(4)/Hf_(3)N_(4) nanocomposites under high pressures is assessed by the in situ synchrotron energy-dispersive X-ray diffraction(ED-XRD)measurements at~19.5 GPa in the temperature range of ca.1000-1900℃.The fracture toughness(K_(IC))of the two-phase nanocomposite amounts~6/6.9 MPa·m^(1/2) and is about 2 times that of single-phaseγ-Si_(3)N_(4),while its hardness of ca.30 GPa remains high.This work provides a reliable and feasible route for the synthesis of advanced hard and tough-Si_(3)N_(4)-based nanocomposites with excellent thermal stabililty.