The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed tw...The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed two co-corresponding authors(Hongxiang Zhang and Honggen Peng).But the corresponding author of Honggen Peng was omitted in the final published manuscript.So,we apply to designate Honggen Peng(penghonggen@ncu.edu.cn)as the second co-corresponding author and the corresponding unit is“a,b">.展开更多
Catalyst design relies heavily on electronic metal‐support interactions,but the metal‐support interface with an uncontrollable electronic or coordination environment makes it challenging.Herein,we outline a promisin...Catalyst design relies heavily on electronic metal‐support interactions,but the metal‐support interface with an uncontrollable electronic or coordination environment makes it challenging.Herein,we outline a promising approach for the rational design of catalysts involving heteroatoms as anchors for Pd nanoparticles for ethanol oxidation reaction(EOR)catalysis.The doped B and N atoms from dimethylamine borane(DB)occupy the position of the Ti_(3)C_(2) lattice to anchor the supported Pd nanoparticles.The electrons transfer from the support to B atoms,and then to the metal Pd to form a stable electronic center.A strong electronic interaction can be produced and the d‐band center can be shifted down,driving Pd into the dominant metallic state and making Pd nanoparticles deposit uniformly on the support.As‐obtained Pd/DB–Ti_(3)C_(2) exhibits superior durability to its counterpart(∼14.6% retention)with 91.1% retention after 2000 cycles,placing it among the top single metal anodic catalysts.Further,in situ Raman and density functional theory computations confirm that Pd/DB–Ti_(3)C_(2) is capable of dehydrogenating ethanol at low reaction energies.展开更多
Efficient yield of^(1)O_(2)determines the photocatalytic degradation rate of antibiotics,but the regulatory mechanism for^(1)O_(2)selective generation in O_(2)activation is still lacking exploration.Herein,oxygen vaca...Efficient yield of^(1)O_(2)determines the photocatalytic degradation rate of antibiotics,but the regulatory mechanism for^(1)O_(2)selective generation in O_(2)activation is still lacking exploration.Herein,oxygen vacancy(OV)modification strategy of MIL-125 was successfully practiced to promote the selective generation of^(1)O_(2).Multiple characterizations including extended X-ray absorption fine structure(EXAFS)and electron paramagnetic resonance spectra(EPR)confirmed the formation of oxygen vacancy in OV-MIL-125.The synthesized OV-MIL-125 exhibited greatly enhanced^(1)O_(2)selective(~90%)and antibiotics removal rate in water with high mineralization rate.Dynamics analysis of excitons by transient-steady state fluorescence and phosphorescence,transient absorption spectra(TAS)revealed that oxygen vacancy greatly enhanced the intersystem crossing(ISC)of singlet exciton,promoting triplet exciton generation.Density functional theoretical(DFT)calculation also proved the reduced gap of intersystem(ΔE_(ST))and the modulated highest occupied molecular orbital(HOMO)-lowest unoccupied molecular orbital(LUMO)population which was conducive to intersystem crossing process.Calculation of transition state further confirmed the lower energy barrier forπ^(*)orbital spin flip of O_(2)adsorbed on OV-MIL-125.The Dexter energy transfer involving triplet annihilation dominated the O_(2)activation mechanism to generate^(1)O_(2)instead of the charge transfer to generate O_(2)^(·-)which happened in MIL-125.This study provides new thinking for photocatalytic activation of molecular oxygen and is expected to guide the design of MOF-based catalysts for water treatment.展开更多
OBJECTIVE: To analyze the component law of Chinese medicines in fuming-washing therapy for knee osteoarthritis(KOA), and develop new fuming-washing prescriptions for KOA through unsupervised data mining methods.METHOD...OBJECTIVE: To analyze the component law of Chinese medicines in fuming-washing therapy for knee osteoarthritis(KOA), and develop new fuming-washing prescriptions for KOA through unsupervised data mining methods.METHODS: Chinese medicine recipes for fuming-washing therapy for KOA were collected and recorded in a database. The correlation coefficient among herbs, core combinations of herbs, andnew prescriptions were analyzed using modified mutual information, complex system entropy cluster, and unsupervised hierarchical clustering, respectively.RESULTS: Based on analysis of 345 Chinese medicine recipes for fuming-washing therapy, 68 herbs occurred frequently, 33 herb pairs occurred frequently, and 12 core combinations were found.Five new fuming-washing recipes for KOA were developed.CONCLUSION: Chinese medicines for fuming-washing therapy of KOA mainly consist of wind-dampness-dispelling and cold-dispersing herbs, blood-activating and stasis-resolving herbs,and wind-dampness-dispelling and heat-clearing herbs. The treatment of fuming-washing therapy for KOA also includes dispelling wind-dampness and dispersing cold, activating blood and resolving stasis, and dispelling wind-dampness and clearing heat. Zhenzhutougucao(Herba Speranskiae Tuberculatae), Honghua(Flos Carthami), Niuxi(Radix Achyranthis Bidentatae), Shenjincao(Herba Lycopodii Japonici), Weilingxian(Radix et Rhizoma Clematidis Chinensis), Chuanwu(Radix Aconiti), Haitongpi(Cortex Erythrinae Variegatae), Ruxiang(Olibanum),Danggui(Radix Angelicae Sinensis), Caowu(Radix Aconiti Kusnezoffii), Moyao(Myrrha), and Aiye(Folium Artemisiae Argyi) are the main herbs used in the fuming-washing treatment for KOA.展开更多
文摘The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed two co-corresponding authors(Hongxiang Zhang and Honggen Peng).But the corresponding author of Honggen Peng was omitted in the final published manuscript.So,we apply to designate Honggen Peng(penghonggen@ncu.edu.cn)as the second co-corresponding author and the corresponding unit is“a,b">.
基金Key Research and Development Program of Zhejiang,Grant/Award Number:2021C03022National Natural Science Foundation of China,Grant/Award Numbers:22002104,22272115,22202145,22202146,22102112,22202147。
文摘Catalyst design relies heavily on electronic metal‐support interactions,but the metal‐support interface with an uncontrollable electronic or coordination environment makes it challenging.Herein,we outline a promising approach for the rational design of catalysts involving heteroatoms as anchors for Pd nanoparticles for ethanol oxidation reaction(EOR)catalysis.The doped B and N atoms from dimethylamine borane(DB)occupy the position of the Ti_(3)C_(2) lattice to anchor the supported Pd nanoparticles.The electrons transfer from the support to B atoms,and then to the metal Pd to form a stable electronic center.A strong electronic interaction can be produced and the d‐band center can be shifted down,driving Pd into the dominant metallic state and making Pd nanoparticles deposit uniformly on the support.As‐obtained Pd/DB–Ti_(3)C_(2) exhibits superior durability to its counterpart(∼14.6% retention)with 91.1% retention after 2000 cycles,placing it among the top single metal anodic catalysts.Further,in situ Raman and density functional theory computations confirm that Pd/DB–Ti_(3)C_(2) is capable of dehydrogenating ethanol at low reaction energies.
基金supported by the National Natural Science Foundation of China(Nos.22276086 and 21976078)the Natural Science Foundation of Jiangxi Province(Nos.20202ACB213001 and20232BAB213029)。
文摘Efficient yield of^(1)O_(2)determines the photocatalytic degradation rate of antibiotics,but the regulatory mechanism for^(1)O_(2)selective generation in O_(2)activation is still lacking exploration.Herein,oxygen vacancy(OV)modification strategy of MIL-125 was successfully practiced to promote the selective generation of^(1)O_(2).Multiple characterizations including extended X-ray absorption fine structure(EXAFS)and electron paramagnetic resonance spectra(EPR)confirmed the formation of oxygen vacancy in OV-MIL-125.The synthesized OV-MIL-125 exhibited greatly enhanced^(1)O_(2)selective(~90%)and antibiotics removal rate in water with high mineralization rate.Dynamics analysis of excitons by transient-steady state fluorescence and phosphorescence,transient absorption spectra(TAS)revealed that oxygen vacancy greatly enhanced the intersystem crossing(ISC)of singlet exciton,promoting triplet exciton generation.Density functional theoretical(DFT)calculation also proved the reduced gap of intersystem(ΔE_(ST))and the modulated highest occupied molecular orbital(HOMO)-lowest unoccupied molecular orbital(LUMO)population which was conducive to intersystem crossing process.Calculation of transition state further confirmed the lower energy barrier forπ^(*)orbital spin flip of O_(2)adsorbed on OV-MIL-125.The Dexter energy transfer involving triplet annihilation dominated the O_(2)activation mechanism to generate^(1)O_(2)instead of the charge transfer to generate O_(2)^(·-)which happened in MIL-125.This study provides new thinking for photocatalytic activation of molecular oxygen and is expected to guide the design of MOF-based catalysts for water treatment.
基金Supported by Grant from the Administration of Traditional Chinese Medicine of Guangdong Province in China(No.20131161)the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20124425110004)
文摘OBJECTIVE: To analyze the component law of Chinese medicines in fuming-washing therapy for knee osteoarthritis(KOA), and develop new fuming-washing prescriptions for KOA through unsupervised data mining methods.METHODS: Chinese medicine recipes for fuming-washing therapy for KOA were collected and recorded in a database. The correlation coefficient among herbs, core combinations of herbs, andnew prescriptions were analyzed using modified mutual information, complex system entropy cluster, and unsupervised hierarchical clustering, respectively.RESULTS: Based on analysis of 345 Chinese medicine recipes for fuming-washing therapy, 68 herbs occurred frequently, 33 herb pairs occurred frequently, and 12 core combinations were found.Five new fuming-washing recipes for KOA were developed.CONCLUSION: Chinese medicines for fuming-washing therapy of KOA mainly consist of wind-dampness-dispelling and cold-dispersing herbs, blood-activating and stasis-resolving herbs,and wind-dampness-dispelling and heat-clearing herbs. The treatment of fuming-washing therapy for KOA also includes dispelling wind-dampness and dispersing cold, activating blood and resolving stasis, and dispelling wind-dampness and clearing heat. Zhenzhutougucao(Herba Speranskiae Tuberculatae), Honghua(Flos Carthami), Niuxi(Radix Achyranthis Bidentatae), Shenjincao(Herba Lycopodii Japonici), Weilingxian(Radix et Rhizoma Clematidis Chinensis), Chuanwu(Radix Aconiti), Haitongpi(Cortex Erythrinae Variegatae), Ruxiang(Olibanum),Danggui(Radix Angelicae Sinensis), Caowu(Radix Aconiti Kusnezoffii), Moyao(Myrrha), and Aiye(Folium Artemisiae Argyi) are the main herbs used in the fuming-washing treatment for KOA.
