Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3...Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3))synthesis.However,the e-NRR performance is currently impeded by the inherent inertness of N_(2) molecules,the extremely slow kinetics and the overwhelming competition from the hydrogen evolution reaction(HER),all of which cause unsatisfied yield and ammonia selectivity(Faradaic efficiency,FE).Defect and interface engineering are capable of achieving novel physical and chemical properties as well as superior synergistic effects for various electrocatalysts.In this review,we first provide a general introduction to the NRR mechanism.We then focus on the recent progress in defect and interface engineering and summarize how defect and interface can be rationally designed and functioned in NRR catalysts.Particularly,the origin of superior NRR catalytic activity by applying these approaches was discussed from both theoretical and experimental perspectives.Finally,the remaining challenges and future perspectives in this emerging area are highlighted.It is expected that this review will shed some light on designing NRR electrocatalysts with excellent activity,selectivity and stability.展开更多
Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnet...Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnetic anisotropy,shows a great potential to increase data storage density for designing magnetic nonvolatile memory and logic devices.However,an electrical control of labyrinthine domain structure remains elusive.Here,we demonstrate the gate-driven evolution of labyrinthine domain structures in an itinerant ferromagnet Cr_(7)Te_(8).By combining electric transport measurements and micromagnetic finite difference simulations,we find that the hysteresis loop of anomalous Hall effect in Cr_(7)Te_(8)samples shows distinct features corresponding to the generation of labyrinthine domain structures.The labyrinthine domain structures are found to be electrically tunable via Li-electrolyte gating,and such gate-driven evolution in Cr_(7)Te_(8)originates from the reduction of the magnetic anisotropic energy with gating,revealed by our micromagnetic simulations.Our results on the gate control of anomalous Hall effect in an itinerant magnetic material provide an opportunity to understand the formation and evolution of labyrinthine domain structures,paving a new route towards electric-field driven spintronics.展开更多
With practical interest in the future applications of next-generation electronic devices,it is imperative to develop new conductive interconnecting materials appropriate for modern electronic devices to replace tradit...With practical interest in the future applications of next-generation electronic devices,it is imperative to develop new conductive interconnecting materials appropriate for modern electronic devices to replace traditional rigid solder tin and silver paste of high melting temperature or corrosive solvent requirements.Herein,we design highly stretchable shape memory self-soldering conductive(SMSC)tape with reversible adhesion switched by temperature,which is composed of silver particles encapsulated by shape memory polymer.SMSC tape has perfect shape and conductivity memory property and anti-fatigue ability even under the strain of 90%.It also exhibits an initial conductivity of 2772 S cm^(−1) and a maximum tensile strain of~100%.The maximum conductivity could be increased to 5446 S cm^(−1) by decreasing the strain to 17%.Meanwhile,SMSC tape can easily realize a heating induced reversible strong-to-weak adhe-sion transition for self-soldering circuit.The combination of stable conductivity,excellent shape memory performance,and temperature-switching reversible adhesion enables SMSC tape to serve two functions of electrode and solder simultaneously.This provides a new way for conductive interconnecting materials to meet requirements of modern electronic devices in the future.展开更多
Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the function...Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the functionalization of LREHs.Although the laminar structures seem to be clear for anion-exchanged compounds,the state of intercalated organic anions and their interactions with cationic rare earth hydroxide layers remain unclear.Herein,we demonstrate that the use of 13C solid-state nuclear magnetic resonance(ssNMR)spectroscopy enables to extract key information on the state of intercalated organic anions such as their local chemical environment,stacking,and dynamics,which are often difficult or impossible to obtain previously.In combination with powder X-ray diffraction and ab initio density functional theory calculations,the intercalation chemistry of two representative layered yttrium hydroxides with selected monovalent organic anions was studied in detail.The products can undergo secondary exchange with a divalent organic anion,depending on the match between the basal spacing of two phases,i.e.,the replacement of benzenesulfonate(BS^(-)),2,4-dimethylbenzene sulfonate(DMBS^(-)),and 4-ethylbenzene sulfonate(EBS)with 2,6-naphthalene disulfonate(NDS^(2-))is allowed due to the insignificant change in basal spacing after exchange,while the replacement of very long dodecyl benzene sulfonate(DBS^(-))and dodecyl sulfate(DS)with NDS^(2-)is forbidden.The results therefore provide valuable insights into the structure-property relationships of LREH-based functional materials.展开更多
基金supported by the National Natural Science Foundation of China(grant no.21904071 and 22071115)。
文摘Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3))synthesis.However,the e-NRR performance is currently impeded by the inherent inertness of N_(2) molecules,the extremely slow kinetics and the overwhelming competition from the hydrogen evolution reaction(HER),all of which cause unsatisfied yield and ammonia selectivity(Faradaic efficiency,FE).Defect and interface engineering are capable of achieving novel physical and chemical properties as well as superior synergistic effects for various electrocatalysts.In this review,we first provide a general introduction to the NRR mechanism.We then focus on the recent progress in defect and interface engineering and summarize how defect and interface can be rationally designed and functioned in NRR catalysts.Particularly,the origin of superior NRR catalytic activity by applying these approaches was discussed from both theoretical and experimental perspectives.Finally,the remaining challenges and future perspectives in this emerging area are highlighted.It is expected that this review will shed some light on designing NRR electrocatalysts with excellent activity,selectivity and stability.
基金supported by the National Natural Science Foundation of China(Grant Nos.92365203,52072168,51861145201,52302180,and 12204232)the National Key Research and Development Program of China(Grant No.2021YFA1202901)+1 种基金the Science and Technology Development Project of Henan Province(Grant No.242102230140)the China Postdoctoral Science Foundation(Grant No.2024M750775)。
文摘Manipulating magnetic domain structure plays a key role in advanced spintronics devices.Theoretical rationale is that the labyrinthine domain structure,normally appearing in ferromagnetic thin films with strong magnetic anisotropy,shows a great potential to increase data storage density for designing magnetic nonvolatile memory and logic devices.However,an electrical control of labyrinthine domain structure remains elusive.Here,we demonstrate the gate-driven evolution of labyrinthine domain structures in an itinerant ferromagnet Cr_(7)Te_(8).By combining electric transport measurements and micromagnetic finite difference simulations,we find that the hysteresis loop of anomalous Hall effect in Cr_(7)Te_(8)samples shows distinct features corresponding to the generation of labyrinthine domain structures.The labyrinthine domain structures are found to be electrically tunable via Li-electrolyte gating,and such gate-driven evolution in Cr_(7)Te_(8)originates from the reduction of the magnetic anisotropic energy with gating,revealed by our micromagnetic simulations.Our results on the gate control of anomalous Hall effect in an itinerant magnetic material provide an opportunity to understand the formation and evolution of labyrinthine domain structures,paving a new route towards electric-field driven spintronics.
基金This work is supported by National Key R&D Program of China(Grant No.2020YFA0711500)the National Natural Science Fund of China(51973095&52011540401).
文摘With practical interest in the future applications of next-generation electronic devices,it is imperative to develop new conductive interconnecting materials appropriate for modern electronic devices to replace traditional rigid solder tin and silver paste of high melting temperature or corrosive solvent requirements.Herein,we design highly stretchable shape memory self-soldering conductive(SMSC)tape with reversible adhesion switched by temperature,which is composed of silver particles encapsulated by shape memory polymer.SMSC tape has perfect shape and conductivity memory property and anti-fatigue ability even under the strain of 90%.It also exhibits an initial conductivity of 2772 S cm^(−1) and a maximum tensile strain of~100%.The maximum conductivity could be increased to 5446 S cm^(−1) by decreasing the strain to 17%.Meanwhile,SMSC tape can easily realize a heating induced reversible strong-to-weak adhe-sion transition for self-soldering circuit.The combination of stable conductivity,excellent shape memory performance,and temperature-switching reversible adhesion enables SMSC tape to serve two functions of electrode and solder simultaneously.This provides a new way for conductive interconnecting materials to meet requirements of modern electronic devices in the future.
基金supported by the National Natural Science Foundation of China(grant no.21904071 and 22071115)the Open Funds(T151904)the State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics of China.
文摘Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the functionalization of LREHs.Although the laminar structures seem to be clear for anion-exchanged compounds,the state of intercalated organic anions and their interactions with cationic rare earth hydroxide layers remain unclear.Herein,we demonstrate that the use of 13C solid-state nuclear magnetic resonance(ssNMR)spectroscopy enables to extract key information on the state of intercalated organic anions such as their local chemical environment,stacking,and dynamics,which are often difficult or impossible to obtain previously.In combination with powder X-ray diffraction and ab initio density functional theory calculations,the intercalation chemistry of two representative layered yttrium hydroxides with selected monovalent organic anions was studied in detail.The products can undergo secondary exchange with a divalent organic anion,depending on the match between the basal spacing of two phases,i.e.,the replacement of benzenesulfonate(BS^(-)),2,4-dimethylbenzene sulfonate(DMBS^(-)),and 4-ethylbenzene sulfonate(EBS)with 2,6-naphthalene disulfonate(NDS^(2-))is allowed due to the insignificant change in basal spacing after exchange,while the replacement of very long dodecyl benzene sulfonate(DBS^(-))and dodecyl sulfate(DS)with NDS^(2-)is forbidden.The results therefore provide valuable insights into the structure-property relationships of LREH-based functional materials.
