Shape-selective zeolites(UZ-x/y) were synthesized by a one-pot method using TPAOH(y) and/or MeEt3 N^+I^-(x) as templates.The use of MeEt3 N^+I^- affects the crystal growth and the distribution of acid sites on the ext...Shape-selective zeolites(UZ-x/y) were synthesized by a one-pot method using TPAOH(y) and/or MeEt3 N^+I^-(x) as templates.The use of MeEt3 N^+I^- affects the crystal growth and the distribution of acid sites on the external surface of the zeolites.The catalysts show excellent catalytic activity towards toluene alkylation with CH3 Br.With toluene conversion of 36.3% and p-xylene selectivity of 66.2%,HZ-40/0 is the most effective among the prepared catalysts,showing a p-xylene yield of 21.2%.The improved para-selectivity is mainly due to the decrease of acid sites on the external surface of the catalysts.展开更多
CO oxidation is a benchmark in heterogeneous catalysis for evaluation of redox catalysts due to its practical relevance in many applications and the fundamental problems associated with its very high activity at low t...CO oxidation is a benchmark in heterogeneous catalysis for evaluation of redox catalysts due to its practical relevance in many applications and the fundamental problems associated with its very high activity at low temperatures.Among which,Co_(3)O_(4) is one of the most active non-precious metal catalysts.Exposed crystal planes and cobalt sites are considered to be important for its high catalytic activity.Herein,we demonstrate an enhanced CO oxidation activity by a defect-rich mesoporous Co_(3)O_(4) that prepared by a designed dual-template method.Two different kinds of silicas are used as hard-templates at the same time,resulting in a defect-rich mesoporous Co_(3)O_(4) with a surface area as high as 169 m^(2)/g.This catalyst exhibited a very high catalytic activity for low temperature CO oxidation with a light-off temperature at -73℃ under the space velocity of 80,000 mL h^(-1)g^(-1)_(cat).Further studies reveal that the high surface area promotes the lattice oxygen mobility,surface rich of Co^(2+)species and active oxygen species are crucial for the high catalytic activity.Moreover,the dual-template approach paves a way towards the design and construction of high-surface-area mesoporous metal oxides for various applications.展开更多
Monolithic catalysts play a crucial role in various catalytic applications,e.g.,chemical synthesis,energy conversion,and environmental treatment,but their catalytic efficiency is often limited by the restricted mass t...Monolithic catalysts play a crucial role in various catalytic applications,e.g.,chemical synthesis,energy conversion,and environmental treatment,but their catalytic efficiency is often limited by the restricted mass transfer and insufficient exposure of active sites.Herein,we present a dual-templating strategy to fabricate atomic Pt dispersed on monolithic N-doped mesoporous carbon nanowires(Pt_(1)/NMCW)with abundant super-/macropores,which,as monolithic catalyst,exhibits high catalytic performance in hydrogenation of 4-nitrophenol(4-NP).During synthesis,triblock copolymer(Pluronic F127)is employed as a primary soft template to generate the mesoporous structured carbon nanowires to improve the accessibility of Pt single sites;KCl crystallite is used as a secondary hard template to create the super-/macropores,which are beneficial for enhancing the mass transfer efficiency.Thanks to the dual-templating strategy that creates the monolithic carbon nanowires with hierarchically porous structure,the obtained Pt_(1)/NMCW shows highly enhanced catalytic activity in 4-NP hydrogenation,outperforming its analogue synthesized without using KCl as template and being comparable to the nano-powder catalyst(i.e.,atomic Pt loaded on the Ndoped carbon nanospheres,Pt_(1)/NCS).展开更多
Aromatic carboxylic acids(ACAs) may be as transformed key metabolites via gut microbiome for playing better pharmacological effects. However, it's rare to achieve high-specificity, high-sensitivity, and highthroug...Aromatic carboxylic acids(ACAs) may be as transformed key metabolites via gut microbiome for playing better pharmacological effects. However, it's rare to achieve high-specificity, high-sensitivity, and highthroughput detection simultaneously, especially, for tracing trace ACAs in gut microbiome. In this work,firstly, a novel dual-template and double-shelled molecularly imprinted 96-well microplates(DDMIPs)was designed and amplified signal for p-hydroxybenzoic acid(PBA) and 3,4,5-trimethoxycinnamic acid(TMA). Additionally, the DDMIPs and a stable isotope labeling derivatization(SILD) method combined with the ultra-high performance liquid chromatography triple quadrupole tandem mass spectrometry(UHPLC-TQ MS) was firstly stepwise integrated, achieving high-effective, high-sensitive, and highthroughput study of gut microbiome metabolism. The whole strategy showed lower limits of detections(LODs) up to 1000 folds than the traditional method, and revealed a more real metabolism-time profile of PBA and TMA by 3-step signal amplification. The platform also laid the foundation for fast, simple,high-selective, high-effective, and high-throughput metabolism and pharmacological research.展开更多
The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report ...The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report a two-step synthesis of 3D ordered mesoporous Cu sphere arrays,which is fabricated by a dual template method using a poly methyl methacrylate(PMMA) inverse opal and the nonionic surfactant Brij 58 to template the mesostructure within the regular voids of a colloidal crystal.Therefo re,the well-ordered 3D interconnected bi-continuous mesopore s structure has advantages of abundant exposed catalytically active sites,efficient mass transport,and high electrical conductivity,which result in excellent electrocatalytic CO2 RR perfo rmance.The prepared 3D ordered mesoporous Cu sphere array(3 D-OMCuSA) exhibits a low onset potential of-0.4 V at a 1 mA cm^-2 electrode current density,a low Tafel slope of 109.6 mV per decade and a long-term durability in 0.1 M potassium bicarbonate.These distinct features of 3 D-OMCuSA render it a promising method for the further develo p ment of advanced electrocatalytic materials for CO2 reduction.展开更多
Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hind...Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hinder the water splitting efficiency.Meanwhile,the high-cost of noble-metal catalysts limit their actual application.It is thus highly urgent to exploit an economical and earthabundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost.Herein,we synthesize the three-dimensionally ordered macro-/mesoporous(3 DOM/m) Ni_(x)Co_(100-x) alloys with distinctive structure and large surface area via a dual-templating technique.Among them,the3 DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm^(2) for HER and OER,respectively.Furthermore,when employed for water splitting,the Ni_(61)Co_(39) only requires 1.60 V to approach 10 mA/cm^(2) and presents excellent stability.These encouraging performances of the Ni_(61)Co_(39) render it a promising bifunctional catalyst for overall water splitting.展开更多
基金Supported by the National Natural Science Foundation of China(21273067,21476065,21671062,21725602)Program for Changjiang Scholars and Innovative Research Team in University(IRT1238)the Fundamental Research Funds for the Central Universities
文摘Shape-selective zeolites(UZ-x/y) were synthesized by a one-pot method using TPAOH(y) and/or MeEt3 N^+I^-(x) as templates.The use of MeEt3 N^+I^- affects the crystal growth and the distribution of acid sites on the external surface of the zeolites.The catalysts show excellent catalytic activity towards toluene alkylation with CH3 Br.With toluene conversion of 36.3% and p-xylene selectivity of 66.2%,HZ-40/0 is the most effective among the prepared catalysts,showing a p-xylene yield of 21.2%.The improved para-selectivity is mainly due to the decrease of acid sites on the external surface of the catalysts.
基金funding from the National Key R&D Program of China (No. 2018YFE0201703)the “1000-Youth Talents Plan”the Fundamental Research Funds for the Central Universities (No. 2042019kf0230)。
文摘CO oxidation is a benchmark in heterogeneous catalysis for evaluation of redox catalysts due to its practical relevance in many applications and the fundamental problems associated with its very high activity at low temperatures.Among which,Co_(3)O_(4) is one of the most active non-precious metal catalysts.Exposed crystal planes and cobalt sites are considered to be important for its high catalytic activity.Herein,we demonstrate an enhanced CO oxidation activity by a defect-rich mesoporous Co_(3)O_(4) that prepared by a designed dual-template method.Two different kinds of silicas are used as hard-templates at the same time,resulting in a defect-rich mesoporous Co_(3)O_(4) with a surface area as high as 169 m^(2)/g.This catalyst exhibited a very high catalytic activity for low temperature CO oxidation with a light-off temperature at -73℃ under the space velocity of 80,000 mL h^(-1)g^(-1)_(cat).Further studies reveal that the high surface area promotes the lattice oxygen mobility,surface rich of Co^(2+)species and active oxygen species are crucial for the high catalytic activity.Moreover,the dual-template approach paves a way towards the design and construction of high-surface-area mesoporous metal oxides for various applications.
基金supported by the National Natural Science Foundation of China(No.21872159)SEI(No.SEI I202134)QIBEBT(No.QIBEBT ZZBS201802).
文摘Monolithic catalysts play a crucial role in various catalytic applications,e.g.,chemical synthesis,energy conversion,and environmental treatment,but their catalytic efficiency is often limited by the restricted mass transfer and insufficient exposure of active sites.Herein,we present a dual-templating strategy to fabricate atomic Pt dispersed on monolithic N-doped mesoporous carbon nanowires(Pt_(1)/NMCW)with abundant super-/macropores,which,as monolithic catalyst,exhibits high catalytic performance in hydrogenation of 4-nitrophenol(4-NP).During synthesis,triblock copolymer(Pluronic F127)is employed as a primary soft template to generate the mesoporous structured carbon nanowires to improve the accessibility of Pt single sites;KCl crystallite is used as a secondary hard template to create the super-/macropores,which are beneficial for enhancing the mass transfer efficiency.Thanks to the dual-templating strategy that creates the monolithic carbon nanowires with hierarchically porous structure,the obtained Pt_(1)/NMCW shows highly enhanced catalytic activity in 4-NP hydrogenation,outperforming its analogue synthesized without using KCl as template and being comparable to the nano-powder catalyst(i.e.,atomic Pt loaded on the Ndoped carbon nanospheres,Pt_(1)/NCS).
基金the National Natural Science Foundation of China (Nos. 82073973, 81872969)the Jilin Provincial Industrial Innovation Special Fund Project (No. 20200703015ZP)the Science and the Youth Innovation Promotion Association of CAS (No. 2019227)。
文摘Aromatic carboxylic acids(ACAs) may be as transformed key metabolites via gut microbiome for playing better pharmacological effects. However, it's rare to achieve high-specificity, high-sensitivity, and highthroughput detection simultaneously, especially, for tracing trace ACAs in gut microbiome. In this work,firstly, a novel dual-template and double-shelled molecularly imprinted 96-well microplates(DDMIPs)was designed and amplified signal for p-hydroxybenzoic acid(PBA) and 3,4,5-trimethoxycinnamic acid(TMA). Additionally, the DDMIPs and a stable isotope labeling derivatization(SILD) method combined with the ultra-high performance liquid chromatography triple quadrupole tandem mass spectrometry(UHPLC-TQ MS) was firstly stepwise integrated, achieving high-effective, high-sensitive, and highthroughput study of gut microbiome metabolism. The whole strategy showed lower limits of detections(LODs) up to 1000 folds than the traditional method, and revealed a more real metabolism-time profile of PBA and TMA by 3-step signal amplification. The platform also laid the foundation for fast, simple,high-selective, high-effective, and high-throughput metabolism and pharmacological research.
基金This work was supported by the NSFC grant number21607113the Natural Science Foundation of Tianjin grant number 17JCQNJC07700。
文摘The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report a two-step synthesis of 3D ordered mesoporous Cu sphere arrays,which is fabricated by a dual template method using a poly methyl methacrylate(PMMA) inverse opal and the nonionic surfactant Brij 58 to template the mesostructure within the regular voids of a colloidal crystal.Therefo re,the well-ordered 3D interconnected bi-continuous mesopore s structure has advantages of abundant exposed catalytically active sites,efficient mass transport,and high electrical conductivity,which result in excellent electrocatalytic CO2 RR perfo rmance.The prepared 3D ordered mesoporous Cu sphere array(3 D-OMCuSA) exhibits a low onset potential of-0.4 V at a 1 mA cm^-2 electrode current density,a low Tafel slope of 109.6 mV per decade and a long-term durability in 0.1 M potassium bicarbonate.These distinct features of 3 D-OMCuSA render it a promising method for the further develo p ment of advanced electrocatalytic materials for CO2 reduction.
基金financially supported by the National Natural Science Foundation of China (No.21676018 and 51172014)。
文摘Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hinder the water splitting efficiency.Meanwhile,the high-cost of noble-metal catalysts limit their actual application.It is thus highly urgent to exploit an economical and earthabundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost.Herein,we synthesize the three-dimensionally ordered macro-/mesoporous(3 DOM/m) Ni_(x)Co_(100-x) alloys with distinctive structure and large surface area via a dual-templating technique.Among them,the3 DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm^(2) for HER and OER,respectively.Furthermore,when employed for water splitting,the Ni_(61)Co_(39) only requires 1.60 V to approach 10 mA/cm^(2) and presents excellent stability.These encouraging performances of the Ni_(61)Co_(39) render it a promising bifunctional catalyst for overall water splitting.