Electrocatalytic CO_(2) reduction(ECR)to high-value fuels and chemicals offers a promising conversion technology for achieving sustainable carbon cycles.In recent years,although great efforts have been made to develop...Electrocatalytic CO_(2) reduction(ECR)to high-value fuels and chemicals offers a promising conversion technology for achieving sustainable carbon cycles.In recent years,although great efforts have been made to develop highefficiency ECR catalysts,challenges remain in achieving high activity and long durability simultaneously.Taking advantage of the adjustable structure,tunable component,and the M–Ch(M¼Sn,In,Bi,etc.,Ch¼S,Se,Te)covalent bonds stabilized metal centers,the p-block metal chalcogenides(PMC)based electrocatalysts have shown great potential in converting CO_(2) into CO or formates.In addition,the unique p-block electron structure can suppress the competitive hydrogen evolution reaction and enhance the adsorption of ECR intermediates.Seeking to systematically understand the structure–activity relationship of PMC-based ECR catalysts,this review summarizes the recent advances in designing PMC electrocatalysts for CO_(2) reduction based on the fundamental aspects of heterogeneous ECR process,including advanced strategies for optimizing the intrinsic activity and improving the loading density of catalytic sites,constructing highly stable catalysts,and tuning product.展开更多
Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an ef...Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an efficient NO_(2)-RR catalyst.Theoretical calculations and in situ electrochemical measurements reveal the creation of Bi1-Ru dual sites which can remarkably promote NO_(2)-activation and suppress proton adsorption,while accelerating the NO_(2)-RR protonation energetics to render a high NO_(2)--to-NH_(3)conversion efficiency.Remarkably,Bi1Ru assembled in a flow cell delivers an NH_(3)yield rate of 1901.4μmol h^(-1)cm^(-2)and an NH_(3)-Faradaic efficiency of 94.3%at an industrial-level current density of 324.3 mA cm^(-2).This study offers new perspectives for designing and constructing p-block single-atom alloys as robust and high-current-density NO_(2)-RR catalysts toward the ammonia electrosynthesis.展开更多
In this paper, we study some actions of a finite group G on the set of characters of its subgroups, and by using these actions we determine the existence of a p-block with given defect group in some cases.
Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures...Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures and tailored functionalization have made MOF materials potential for applications in many fields. Among various MOF materials, 3p-block metal(Al, Ga, and In)-based MOFs exhibit higher chemical stability than divalent transition metal-based MOFs due to their higher valence. In this review, Al-MOFs and In-MOFs were mainly discussed from the perspective of categories of inorganic building blocks, coordination types, and numbers of organic ligands. This review will give intuitive guidance to the design and synthesis of novel 3p-block metal-based MOFs with potential applications.展开更多
p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been ex...p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been extensively studied.The effects of synthesis conditions on the photocatalytic activity were discussed.The Sr_(1.36)Sb_(2)O_(6)-100°C-24 h-5 and Sr_(2)Sb_(2)O_(7)-150℃-24 h^(-2) samples prepared under optimal conditions exhibited remarkably different photocatalytic activities.The essential factors influencing the difference of photocatalytic performance were revealed.The results showed that the different photocatalytic activities observed for Sr_(1.36)Sb_(2)O_(6)and Sr_(2)Sb_(2)O_(7) could be attributed to their different electronic and crystal structures.Our work will provide a new perspective for the screening and design of p-block metal composite oxide photocatalysts to enhance the removal of organic pollutants in the environment.展开更多
多输入多输出(Multiple-Input Multiple-Output,MIMO)雷达在阵元故障时虚拟阵列输出数据矩阵会出现大量的整行数据丢失,由于阵列接收数据矩阵的不完整而导致对波达方向(Direction of Arrival,DOA)的估计性能恶化。大多数低秩矩阵填充算...多输入多输出(Multiple-Input Multiple-Output,MIMO)雷达在阵元故障时虚拟阵列输出数据矩阵会出现大量的整行数据丢失,由于阵列接收数据矩阵的不完整而导致对波达方向(Direction of Arrival,DOA)的估计性能恶化。大多数低秩矩阵填充算法要求缺失数据随机分布于不完整的矩阵中,无法适用于整行缺失数据的恢复问题。为此,提出了一种基于低秩块Hankel矩阵正则化的阵元故障MIMO雷达DOA估计方法。首先,通过奇异值分解(Singular Value Decomposition,SVD)降低虚拟阵列输出矩阵的维度,以减少计算复杂度。然后,对降维数据矩阵建立基于块Hankel矩阵正则化的低秩矩阵填充模型,在该模型中将MIMO雷达降维数据矩阵排列成块Hankel矩阵并施加Schatten-p范数作为正则项。最后,结合交替方向乘子法(Alternate Direction Multiplier Method,ADMM)求解该模型,获得完整的MIMO雷达降维数据矩阵。仿真结果表明,所提方法能够有效恢复降维数据矩阵中的整行数据缺失,具有较高的DOA估计精度和实时性,在阵元故障率低于50.0%时DOA估计精度优于现有方法。展开更多
The fixation and conversion of CO_(2)frommedium-and high-temperature industrial exhaust gases arescientifically important and challenging tasks owing to theharsh conditions required.Ga_(2)O_(3),a stable p-block compou...The fixation and conversion of CO_(2)frommedium-and high-temperature industrial exhaust gases arescientifically important and challenging tasks owing to theharsh conditions required.Ga_(2)O_(3),a stable p-block compound,is surprisingly active in the thermal conversion of hot CO_(2)waste gas,but its underlying mechanism remains unclear.Inthis study,we investigated CO_(2)adsorption and activationacross 11 different Ga_(2)O_(3)-terminated faces using densityfunctional theory.Charge transfer and chemical bond analysesrevealed the occurrence of two distinct activation mechanismsinvolving synchronous electron gain and loss,driven by astrong synergetic effect between Ga cations and O anions onthe substrate surface.This Ga-O synergy enhances the CO_(2)activation efficiency compared with single active sites,with CO_(2)^(δ+) cation more readily capturing H atom than CO_(2)^(δ–).Tothe best of our knowledge,such a dual activation mechanismhas not been reported before,particularly for p-block catalysts.Our findings provide new insights into the direct catalyticconversion of CO_(2)emissions and offer strategies for the rational design of industrial-grade catalysts for medium-andhigh-temperature CO_(2)tail gas conversion.展开更多
基金support from the National Key Research and Development Program of China(No.2020YFB1505801)the National Natural Science Foundation of China(Nos.22025208,22075300,and 22102191)the Chinese Academy of Sciences,and the Key Laboratory of Education department of Shaanxi Province(20JS157).
文摘Electrocatalytic CO_(2) reduction(ECR)to high-value fuels and chemicals offers a promising conversion technology for achieving sustainable carbon cycles.In recent years,although great efforts have been made to develop highefficiency ECR catalysts,challenges remain in achieving high activity and long durability simultaneously.Taking advantage of the adjustable structure,tunable component,and the M–Ch(M¼Sn,In,Bi,etc.,Ch¼S,Se,Te)covalent bonds stabilized metal centers,the p-block metal chalcogenides(PMC)based electrocatalysts have shown great potential in converting CO_(2) into CO or formates.In addition,the unique p-block electron structure can suppress the competitive hydrogen evolution reaction and enhance the adsorption of ECR intermediates.Seeking to systematically understand the structure–activity relationship of PMC-based ECR catalysts,this review summarizes the recent advances in designing PMC electrocatalysts for CO_(2) reduction based on the fundamental aspects of heterogeneous ECR process,including advanced strategies for optimizing the intrinsic activity and improving the loading density of catalytic sites,constructing highly stable catalysts,and tuning product.
基金Longyuan Youth Innovative and Entrepreneurial Talents ProjectProgram for Top Leading Talents of Gansu Province。
文摘Electrochemical reduction of NO_(2)-to NH_(3)(NO_(2)-RR) is recognized as an appealing approach for achieving renewable NH_(3)synthesis and waste NO_(2)-removal.Herein,we report isolated Bi alloyed Ru (Bi1Ru) as an efficient NO_(2)-RR catalyst.Theoretical calculations and in situ electrochemical measurements reveal the creation of Bi1-Ru dual sites which can remarkably promote NO_(2)-activation and suppress proton adsorption,while accelerating the NO_(2)-RR protonation energetics to render a high NO_(2)--to-NH_(3)conversion efficiency.Remarkably,Bi1Ru assembled in a flow cell delivers an NH_(3)yield rate of 1901.4μmol h^(-1)cm^(-2)and an NH_(3)-Faradaic efficiency of 94.3%at an industrial-level current density of 324.3 mA cm^(-2).This study offers new perspectives for designing and constructing p-block single-atom alloys as robust and high-current-density NO_(2)-RR catalysts toward the ammonia electrosynthesis.
文摘In this paper, we study some actions of a finite group G on the set of characters of its subgroups, and by using these actions we determine the existence of a p-block with given defect group in some cases.
基金This work was supported by the National Natural Science Foundation of China(No. 21771078).
文摘Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures and tailored functionalization have made MOF materials potential for applications in many fields. Among various MOF materials, 3p-block metal(Al, Ga, and In)-based MOFs exhibit higher chemical stability than divalent transition metal-based MOFs due to their higher valence. In this review, Al-MOFs and In-MOFs were mainly discussed from the perspective of categories of inorganic building blocks, coordination types, and numbers of organic ligands. This review will give intuitive guidance to the design and synthesis of novel 3p-block metal-based MOFs with potential applications.
基金financially supported by the National Natural Science Foundation of China(21875037,51502036)the National Key Research and Development Program of China(2016YFB0302303,2019YFC1908203)the Natural Science Foundation of Distinguished Young Scholars of Fujian Province(2019J06015)。
文摘p-block metal composite oxides Sr_(1.36)Sb_(2)O_(6) and Sr_(2)Sb_(2)O_(7) synthesized by a hydrothermal method as photocatalysts in the degradation of tetracycline hydrochloride under UV light irradiation have been extensively studied.The effects of synthesis conditions on the photocatalytic activity were discussed.The Sr_(1.36)Sb_(2)O_(6)-100°C-24 h-5 and Sr_(2)Sb_(2)O_(7)-150℃-24 h^(-2) samples prepared under optimal conditions exhibited remarkably different photocatalytic activities.The essential factors influencing the difference of photocatalytic performance were revealed.The results showed that the different photocatalytic activities observed for Sr_(1.36)Sb_(2)O_(6)and Sr_(2)Sb_(2)O_(7) could be attributed to their different electronic and crystal structures.Our work will provide a new perspective for the screening and design of p-block metal composite oxide photocatalysts to enhance the removal of organic pollutants in the environment.
文摘多输入多输出(Multiple-Input Multiple-Output,MIMO)雷达在阵元故障时虚拟阵列输出数据矩阵会出现大量的整行数据丢失,由于阵列接收数据矩阵的不完整而导致对波达方向(Direction of Arrival,DOA)的估计性能恶化。大多数低秩矩阵填充算法要求缺失数据随机分布于不完整的矩阵中,无法适用于整行缺失数据的恢复问题。为此,提出了一种基于低秩块Hankel矩阵正则化的阵元故障MIMO雷达DOA估计方法。首先,通过奇异值分解(Singular Value Decomposition,SVD)降低虚拟阵列输出矩阵的维度,以减少计算复杂度。然后,对降维数据矩阵建立基于块Hankel矩阵正则化的低秩矩阵填充模型,在该模型中将MIMO雷达降维数据矩阵排列成块Hankel矩阵并施加Schatten-p范数作为正则项。最后,结合交替方向乘子法(Alternate Direction Multiplier Method,ADMM)求解该模型,获得完整的MIMO雷达降维数据矩阵。仿真结果表明,所提方法能够有效恢复降维数据矩阵中的整行数据缺失,具有较高的DOA估计精度和实时性,在阵元故障率低于50.0%时DOA估计精度优于现有方法。
基金supported by the Key Research and Development Program of Hubei Province(2023BAB032)the Chaozhou Ceramic Industry Talent Revitalization Plan-Talent Support Project for Basic Research Platform of Ceramic Material Application+1 种基金the Self-Innovation Research Funding Project of Hanjiang Laboratory(HJL2023001)the Hubei Provincial Natural Science Foundation of China(2023AFB1000)。
文摘The fixation and conversion of CO_(2)frommedium-and high-temperature industrial exhaust gases arescientifically important and challenging tasks owing to theharsh conditions required.Ga_(2)O_(3),a stable p-block compound,is surprisingly active in the thermal conversion of hot CO_(2)waste gas,but its underlying mechanism remains unclear.Inthis study,we investigated CO_(2)adsorption and activationacross 11 different Ga_(2)O_(3)-terminated faces using densityfunctional theory.Charge transfer and chemical bond analysesrevealed the occurrence of two distinct activation mechanismsinvolving synchronous electron gain and loss,driven by astrong synergetic effect between Ga cations and O anions onthe substrate surface.This Ga-O synergy enhances the CO_(2)activation efficiency compared with single active sites,with CO_(2)^(δ+) cation more readily capturing H atom than CO_(2)^(δ–).Tothe best of our knowledge,such a dual activation mechanismhas not been reported before,particularly for p-block catalysts.Our findings provide new insights into the direct catalyticconversion of CO_(2)emissions and offer strategies for the rational design of industrial-grade catalysts for medium-andhigh-temperature CO_(2)tail gas conversion.
