Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer...Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.展开更多
The achievement of electrical spin control is highly desirable.One promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its...The achievement of electrical spin control is highly desirable.One promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its Rashba constant to external electric fields holds great potential for short channel lengths in spin field-effect transistors,which is crucial for preserving spin coherence and enhancing integration density.Hence,two-dimensional(2D)Rashba semiconductors with large Rashba constants and significant electric field responses are highly desirable.Herein,by employing first-principles calculations,we design a thermodynamically stable 2D Rashba semiconductor,YSbTe_(3),which possesses an indirect band gap of 1.04 eV,a large Rashba constant of 1.54 eV·Åand a strong electric field response of up to 4.80 e·Å^(2).In particular,the Rashba constant dependence on the electric field shows an unusual nonlinear relationship.At the same time,YSbTe_(3)has been identified as a 2D ferroelectric material with a moderate polarization switching energy barrier(~0.33 eV per formula).By changing the electric polarization direction,the Rashba spin texture of YSbTe_(3)can be reversed.These out-standing properties make the ferroelectric Rashba semiconductor YSbTe_(3)quite promising for spintronic applications.展开更多
Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,t...Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.展开更多
In order to inhibit hydrogen evolution and enhance current efficiency of Zn-Fe alloy electrodeposition from alkaline zincate solution, hydrogen inhibitors composed of the sulfur group elements were optimized on the ba...In order to inhibit hydrogen evolution and enhance current efficiency of Zn-Fe alloy electrodeposition from alkaline zincate solution, hydrogen inhibitors composed of the sulfur group elements were optimized on the basis of atom structures analysis. The effects of hydrogen inhibitor on the current efficiency of Zn-Fe alloy electroplating and their electrochemical behaviors were studied. The results indicate that hydrogen inhibitor can increase the current efficiency of Zn-Fe alloy electroplating evidently, from 63.28% without hydrogen inhibitor up to 83.54% with a hydrogen inhibitor at a volume fraction of 2.0%, while it has a minor influence on that of pure Zn plating, which maintains at 80%. The optimum volume fraction of hydrogen inhibitor is 2.0%.展开更多
The action between imidazolinyl-quaternary-ammonium-salt(IQAS) molecule and Fe atom was studied, and the influence of the alkyl group connected with N atom of imidazoline ring on corrosion inhibition efficiency was ex...The action between imidazolinyl-quaternary-ammonium-salt(IQAS) molecule and Fe atom was studied, and the influence of the alkyl group connected with N atom of imidazoline ring on corrosion inhibition efficiency was explored. Quantum chemical methods, HF/6-31 G and HF/Lan L2 dz, were applied successively to calculate the parameters such as front molecular orbit energy of IQASⅠ-Ⅳ and chemical adsorption for IQASⅠ-Ⅳ and Fe atom. The corrosion inhibition efficiency was measured with the weight loss method of carbon steel samples in acidic solution and oil field sewage. Based on the theoretical analyses and experimental results, it is concluded that N-Fe coordination bond is formed between IQAS molecule and Fe atom, corrosion inhibition efficiency is decreased in the following order(from large to small): IQAS Ⅳ, IQAS Ⅲ, IQAS Ⅱ, IQASⅠ.展开更多
The combustion process of pulverized coal injected into blast furnace involves a lot of physical and chemical reactions. Based on the combustion behaviors of pulverized coal, the conception of coal effective calorific...The combustion process of pulverized coal injected into blast furnace involves a lot of physical and chemical reactions. Based on the combustion behaviors of pulverized coal, the conception of coal effective calorific value representing the actual thermal energy provided for blast furnace was proposed. A cost performance evaluation model of coal injection was built up for the optimal selection of various kinds of coal based on effective calorific value. The model contains two indicators: coal effective calorific value which has eight sub-indicators and coal injection cost which includes four sub-indicators. In addition, the calculation principle and application of cost performance evaluation model in a Chinese large-scale iron and steel company were comprehensively introduced. The evaluation results finally confirm that this novel model is of great significance to the optimal selection of blast furnace pulverized coal.展开更多
Malachite,being highly hydrophilic and difficult to be floated conventionally,is usually beneficiated by sulfidation flotation in industry.However,the complex crystal structure of malachite leads to the formation of v...Malachite,being highly hydrophilic and difficult to be floated conventionally,is usually beneficiated by sulfidation flotation in industry.However,the complex crystal structure of malachite leads to the formation of various fracture surfaces with distinct properties during crushing and grinding,resulting in surface anisotropy.In this study,we explored the surface anisotropy of malachite and further investigated its sulfidation mechanism from the coordination chemistry perspective,considering the influence of the Jahn-Teller effect on malachite sulfidation.Computational results reveal that the penta-coordinated Cu ions on the malachite(201)and(010)surfaces exhibit stronger activity compared to those on the malachite(201)surface.Additionally,the tetra-coordinated structure formed by HS^(−)adsorption on the malachite(010)and(201)surfaces is more stable,with more negative adsorption energy,compared to the hexa coordinated structure formed by HS−adsorption on the(201)surface.The sulfidized malachite surface has an additional pair ofπelectron and smaller HOMO(highest occupied molecular orbital)-LUMO(lowest unoccupied molecular orbital)gap with xanthate molecules,causing strongerπbackbonding with xanthate.This study provides new insights into the surface sulfidation mechanism of malachite and offers a theoretical reference for the design of targeted flotation reagents.展开更多
基金supported by the National Key Research and Development Program of China(2021YFA1500500,2019-YFA0405600)the CAS Project for Young Scientists in Basic Research(YSBR-051)+6 种基金the National Science Fund for Distinguished Young Scholars(21925204)the National Natural Science Foundation of China(22202192,U19A2015,22221003,22250007,22163002)the Collaborative Innovation Program of Hefei Science Center,CAS(2022HSCCIP004)the International Partnership,the DNL Cooperation Fund,CAS(DNL202003)the USTC Research Funds of the Double First-Class Initiative(YD9990002016,YD999000-2014)the Program of Chinese Academy of Sciences(123GJHZ2022101GC)the Fundamental Research Funds for the Central Universities(WK9990000095,WK999000-0124).
文摘Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.
基金supported by the National Natural Science Foundation of China(22322304,22273092,22373095)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450101)+2 种基金the Innovation Program for Quantum Science and Technology(2021ZD0303306)the USTC Tang ScholarThe authors wish to acknowledge the Supercomputing Center of the USTC for providing computational resources.
文摘The achievement of electrical spin control is highly desirable.One promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its Rashba constant to external electric fields holds great potential for short channel lengths in spin field-effect transistors,which is crucial for preserving spin coherence and enhancing integration density.Hence,two-dimensional(2D)Rashba semiconductors with large Rashba constants and significant electric field responses are highly desirable.Herein,by employing first-principles calculations,we design a thermodynamically stable 2D Rashba semiconductor,YSbTe_(3),which possesses an indirect band gap of 1.04 eV,a large Rashba constant of 1.54 eV·Åand a strong electric field response of up to 4.80 e·Å^(2).In particular,the Rashba constant dependence on the electric field shows an unusual nonlinear relationship.At the same time,YSbTe_(3)has been identified as a 2D ferroelectric material with a moderate polarization switching energy barrier(~0.33 eV per formula).By changing the electric polarization direction,the Rashba spin texture of YSbTe_(3)can be reversed.These out-standing properties make the ferroelectric Rashba semiconductor YSbTe_(3)quite promising for spintronic applications.
文摘Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.
基金Project(50274073) supported by the National Natural Science Foundation of China
文摘In order to inhibit hydrogen evolution and enhance current efficiency of Zn-Fe alloy electrodeposition from alkaline zincate solution, hydrogen inhibitors composed of the sulfur group elements were optimized on the basis of atom structures analysis. The effects of hydrogen inhibitor on the current efficiency of Zn-Fe alloy electroplating and their electrochemical behaviors were studied. The results indicate that hydrogen inhibitor can increase the current efficiency of Zn-Fe alloy electroplating evidently, from 63.28% without hydrogen inhibitor up to 83.54% with a hydrogen inhibitor at a volume fraction of 2.0%, while it has a minor influence on that of pure Zn plating, which maintains at 80%. The optimum volume fraction of hydrogen inhibitor is 2.0%.
基金Project (05A002) supported by Scientific Research Fundation of Hunan Provincial Education Depart ment project(04JJY40010) supported by the Natural Science Foundation of Hunan Province
文摘The action between imidazolinyl-quaternary-ammonium-salt(IQAS) molecule and Fe atom was studied, and the influence of the alkyl group connected with N atom of imidazoline ring on corrosion inhibition efficiency was explored. Quantum chemical methods, HF/6-31 G and HF/Lan L2 dz, were applied successively to calculate the parameters such as front molecular orbit energy of IQASⅠ-Ⅳ and chemical adsorption for IQASⅠ-Ⅳ and Fe atom. The corrosion inhibition efficiency was measured with the weight loss method of carbon steel samples in acidic solution and oil field sewage. Based on the theoretical analyses and experimental results, it is concluded that N-Fe coordination bond is formed between IQAS molecule and Fe atom, corrosion inhibition efficiency is decreased in the following order(from large to small): IQAS Ⅳ, IQAS Ⅲ, IQAS Ⅱ, IQASⅠ.
基金Project(51134008)supported by the National Natural Science Foundation of ChinaProject(2012CB720401)supported by the National Basic Research Program of China
文摘The combustion process of pulverized coal injected into blast furnace involves a lot of physical and chemical reactions. Based on the combustion behaviors of pulverized coal, the conception of coal effective calorific value representing the actual thermal energy provided for blast furnace was proposed. A cost performance evaluation model of coal injection was built up for the optimal selection of various kinds of coal based on effective calorific value. The model contains two indicators: coal effective calorific value which has eight sub-indicators and coal injection cost which includes four sub-indicators. In addition, the calculation principle and application of cost performance evaluation model in a Chinese large-scale iron and steel company were comprehensively introduced. The evaluation results finally confirm that this novel model is of great significance to the optimal selection of blast furnace pulverized coal.
基金Projects(52074356,U22A20170)supported by the National Natural Science Foundation of ChinaProject(2022YFC2904503)supported by the National Key R&D Program of China+4 种基金Project(2023SK2061)supported by the Special Fund for the Construction of Hunan Innovative Province,ChinaProject(2023CXQD002)supported by the Innovation-driven Project of Central South University,ChinaProject(2022RC1183)supported by the Science and Technology Innovation Program of Hunan Province,ChinaProject(kq2009005)supported by the Changsha Science and Technology Project(Changsha Outstanding Innovative Youth Training Program),ChinaProject supported by the High-performance Computing Centers of Central South University,China。
文摘Malachite,being highly hydrophilic and difficult to be floated conventionally,is usually beneficiated by sulfidation flotation in industry.However,the complex crystal structure of malachite leads to the formation of various fracture surfaces with distinct properties during crushing and grinding,resulting in surface anisotropy.In this study,we explored the surface anisotropy of malachite and further investigated its sulfidation mechanism from the coordination chemistry perspective,considering the influence of the Jahn-Teller effect on malachite sulfidation.Computational results reveal that the penta-coordinated Cu ions on the malachite(201)and(010)surfaces exhibit stronger activity compared to those on the malachite(201)surface.Additionally,the tetra-coordinated structure formed by HS^(−)adsorption on the malachite(010)and(201)surfaces is more stable,with more negative adsorption energy,compared to the hexa coordinated structure formed by HS−adsorption on the(201)surface.The sulfidized malachite surface has an additional pair ofπelectron and smaller HOMO(highest occupied molecular orbital)-LUMO(lowest unoccupied molecular orbital)gap with xanthate molecules,causing strongerπbackbonding with xanthate.This study provides new insights into the surface sulfidation mechanism of malachite and offers a theoretical reference for the design of targeted flotation reagents.
