Although the simple adaptive control （SAC） is widely studied both in theory and application in flexible space structure control and other control problems, it is restricted by the almost strictly positive real （ASP...Although the simple adaptive control （SAC） is widely studied both in theory and application in flexible space structure control and other control problems, it is restricted by the almost strictly positive real （ASPR） conditions. In most practical control problems, the ASPR conditions are not satisfied. Therefore, based on the SAC theory, this paper proposes a backstepping simple adaptive control algorithm which suits the system with arbitrary relative degree with no need of parallel feed forward compensa- tor. The proposed control algorithm consists of decomposition of the arbitrary relative degree system into a known subsystem and an unknown ASPR subsystem which are connected in cascade, design of constant output feedback controller for the known subsystem, and implementation of backstepping method and SAC of the unknown ASPR subsystem. Inheriting the characteristics of the SAC, this method can be adaptive online for the parameter uncertainties. Then, the application of the proposed controller to large flexible space structure with collocated sensors and actuators is studied, and the simulation results validate the proposed controller. It is a new strategy to apply the classical SAC to high relative degree plants.展开更多
Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction int...Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst.Here,a family of n%-Co_(3)O_(4)/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co^(2+)and Co^(3+)were prepared for NO_(3)RR.We found that Co^(3+)primarily acts as the active site for NO_(3)^(−)reduction to NO_(2)^(−),while Co^(2+)is responsible for the conversion of NO_(2)^(−)to NH_(3).Moreover,the conversion of these intermediates over the active sites is autonomous and separately controllable.Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia.Combining the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(^(*)NHO→^(*)NHOH→^(*)NH_(2)OH→^(*)NH_(2)→^(*)NH_(3))is more favorable due to the lowerΔG value(0.25 eV)for the rate-limiting step(^(*)NO→^(*)NHO).The NH_(3)yield rate of 8%-Co_(3)O_(4)/SiC reached 1.08 mmol/(cm^(2)h)with a Faradaic efficiency of 96.4%at−0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO_(3)RR catalysts.This strategy not only provides an efficient catalyst for NO_(3)RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.展开更多
The pervasive accumulation of plastic waste exacerbates environmental degradation and undermines resource circularity.Selective thermal catalysis emerges as a transformative pathway for valorizing waste plastics into ...The pervasive accumulation of plastic waste exacerbates environmental degradation and undermines resource circularity.Selective thermal catalysis emerges as a transformative pathway for valorizing waste plastics into value-added chemicals,yet persistent challenges in catalytic activity and product selectivity demand systematic resolution.This review decodes cutting-edge advances in thermal depolymerization by converging two critical dimensions:atomic-scale active site engineering-where rational design of coordination features and interfacial architectures regulates C-C cleavage energetics and intermediate adsorption-and macromolecular-scale manipulation of polymer transient states-leveraging nanoconfinement effects,chain folding dynamics,and thermal fragmentation to accelerate conversion kinetics.We further highlight breakthroughs in operando char-acterization techniques that resolve time-evolving reaction coordinates across catalytic systems.By establishing multiscale structure-activity relationships linking catalyst configurations to polymer dynamics,this analysis derives design paradigms for next-generation upcycling systems.These principles enable economically viable,industrially scalable plastic valorization while charting a strategic trajectory toward carbon-circular economies.展开更多
基金National Natural Science Foundation of China(10902003)
文摘Although the simple adaptive control （SAC） is widely studied both in theory and application in flexible space structure control and other control problems, it is restricted by the almost strictly positive real （ASPR） conditions. In most practical control problems, the ASPR conditions are not satisfied. Therefore, based on the SAC theory, this paper proposes a backstepping simple adaptive control algorithm which suits the system with arbitrary relative degree with no need of parallel feed forward compensa- tor. The proposed control algorithm consists of decomposition of the arbitrary relative degree system into a known subsystem and an unknown ASPR subsystem which are connected in cascade, design of constant output feedback controller for the known subsystem, and implementation of backstepping method and SAC of the unknown ASPR subsystem. Inheriting the characteristics of the SAC, this method can be adaptive online for the parameter uncertainties. Then, the application of the proposed controller to large flexible space structure with collocated sensors and actuators is studied, and the simulation results validate the proposed controller. It is a new strategy to apply the classical SAC to high relative degree plants.
基金financially supported by the National Key Research and Development Program of China (2018YFA0209404)the Fundamental Research Funds for the Central Universities (DUT22LAB601)
文摘Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst.Here,a family of n%-Co_(3)O_(4)/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co^(2+)and Co^(3+)were prepared for NO_(3)RR.We found that Co^(3+)primarily acts as the active site for NO_(3)^(−)reduction to NO_(2)^(−),while Co^(2+)is responsible for the conversion of NO_(2)^(−)to NH_(3).Moreover,the conversion of these intermediates over the active sites is autonomous and separately controllable.Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia.Combining the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(^(*)NHO→^(*)NHOH→^(*)NH_(2)OH→^(*)NH_(2)→^(*)NH_(3))is more favorable due to the lowerΔG value(0.25 eV)for the rate-limiting step(^(*)NO→^(*)NHO).The NH_(3)yield rate of 8%-Co_(3)O_(4)/SiC reached 1.08 mmol/(cm^(2)h)with a Faradaic efficiency of 96.4%at−0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO_(3)RR catalysts.This strategy not only provides an efficient catalyst for NO_(3)RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.
基金supported by the Key Technologies Research and Development Program(2024YFC2909605)Black Soil Project of Shenyang Science and Technology Program(24-216-2-07)Fundamental Research Funds for the Central Universities(NO.N25BSS006).
文摘The pervasive accumulation of plastic waste exacerbates environmental degradation and undermines resource circularity.Selective thermal catalysis emerges as a transformative pathway for valorizing waste plastics into value-added chemicals,yet persistent challenges in catalytic activity and product selectivity demand systematic resolution.This review decodes cutting-edge advances in thermal depolymerization by converging two critical dimensions:atomic-scale active site engineering-where rational design of coordination features and interfacial architectures regulates C-C cleavage energetics and intermediate adsorption-and macromolecular-scale manipulation of polymer transient states-leveraging nanoconfinement effects,chain folding dynamics,and thermal fragmentation to accelerate conversion kinetics.We further highlight breakthroughs in operando char-acterization techniques that resolve time-evolving reaction coordinates across catalytic systems.By establishing multiscale structure-activity relationships linking catalyst configurations to polymer dynamics,this analysis derives design paradigms for next-generation upcycling systems.These principles enable economically viable,industrially scalable plastic valorization while charting a strategic trajectory toward carbon-circular economies.
