催化氧化技术是治理挥发性有机物(VOCs)的有效手段,其中新型催化剂的设计与优化是实现VOCs高效转化的关键。分别采用焙烧法与沉淀法制备了CeO_(2)活性载体,随后通过硼氢化钠还原法将Pt负载于CeO_(2)表面制备了Pt/CeO_(2)催化剂,进而考...催化氧化技术是治理挥发性有机物(VOCs)的有效手段,其中新型催化剂的设计与优化是实现VOCs高效转化的关键。分别采用焙烧法与沉淀法制备了CeO_(2)活性载体,随后通过硼氢化钠还原法将Pt负载于CeO_(2)表面制备了Pt/CeO_(2)催化剂,进而考察了不同制备方法对其催化氧化甲苯性能的影响。通过XRD、N_(2)吸/脱附、紫外拉曼光谱、XPS及O_(2)-TPD等手段对催化剂进行了表征。通过in situ DRIFTS研究了甲苯在反应过程中的演变行为。结果表明,不同制备方法均调控了Pt/CeO_(2)催化剂中活性氧物种的浓度。其中,沉淀-还原法制备的Pt/CeO_(2)-P催化剂具有更高的活性氧物种和氧空位浓度,促进了甲苯的活化与转化,使其生成易于降解的甲酸盐物种,并最终氧化为CO_(2)和H_(2)O。在甲苯浓度(体积分数)为0.1%、空速为48000 m L/(g·h)条件下,Pt/CeO_(2)-P催化剂的T50和T90(甲苯转化率达到50%和90%时的反应温度)分别低至157℃和168℃。展开更多
Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious ...Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious metal ions,V_(2)O_(3)spiny hollow nanospheres(pV_(2)O_(3)SHN),was synthe sized through a one-step hydrothermal-as sis ted methodology for the adsorption of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) from the leaching solution of electronic waste.The results reveal that the p-V2O3SHN hierarchy was successfully constructed with a hollow structure and dense spiny morphology.The prepared p-V2O3SHN can effectively remove precious metal ions such as Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ),with the selective capture order being Au(Ⅲ)> Ag(Ⅰ)> Pt(Ⅳ)> Pd(Ⅱ)> other metal ions.This superior adsorption capability can be attributed to the multi-diffusible,intermingled composition,and numerous active sites decorating the p-V2O3SHN hierarchy,facilitating the uptake of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) ions from electronic waste.The Langmuir model provided a better fit for the uptake process,revealing maximum uptake capacities of 833.33 mg/g for Au(Ⅲ),370.37 mg/g for Ag(Ⅰ),42.01 mg/g for Pd(Ⅱ),and 77.51 mg/g for Pt(Ⅳ) on p-V_(2)O_(3)SHN.Remarkably,p-V_(2)O_(3)SHN exhibited a robust affinity for the adsorbate due to the presence of surface defects and reduction reactions.The new p-V2O3SHN also demonstrated good reusability for three sorption cycles,highlighting its potential for electronic waste treatment.Due to its facile synthesis and excellent efficiency,hierarchical p-V2O3SHN presents itself as a promising candidate for the selective uptake of Au(Ⅲ),Ag(Ⅰ),Pt(Ⅳ),and Pd(Ⅱ) from electronic waste.展开更多
The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batterie...The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batteries.To improve the reaction kinetics and decrease the reaction overpotential,we synthesized mesoporous Pt nanosheets with high tensile strain.The presence of many unsaturated coordinated Pt atoms around the pores gives rise to tensile strain in the mesoporous Pt nanosheets.This tensile strain plays a key role in regulating the interactions between the catalytic surface of Pt and the adsorbed intermediates.The two-dimensional structure provides more active sites on the surface for the catalytic reactions.These superiorities enable a low overpotential of 0.36 V at a cutoff capacity of 100μAh·cm^(−2) at a current density of 10μA·cm^(−2) over more than 2000 h.This study opens new possibilities for the rational design of metal-based materials with strain engineering for electrochemical energy storage.展开更多
Catalytic oxidation is an effective strategy for eliminating CO pollutant.Pt/TiO_(2) catalyst are one of the most active catalysts as used,but facing the issue of sulfur and water deactivation.In this study,TiO_(2) wa...Catalytic oxidation is an effective strategy for eliminating CO pollutant.Pt/TiO_(2) catalyst are one of the most active catalysts as used,but facing the issue of sulfur and water deactivation.In this study,TiO_(2) was synthesized using a sol-gel method,while Pt/TiO_(2) was prepared by impregnation method.By varying the calcination temperature of the TiO_(2) support,Pt/TiO_(2) catalysts with different proportions of anatase and rutile phases were synthesized.At the calcination temperature of 500℃,the catalysts exhibited approximately equal proportions of anatase and rutile,resulting in exceptional catalytic activity for CO oxidation,as well as improved resistance to sulfur and water in the flue gas.Consequently,the Pt/TiO_(2)-500 catalyst achieved a CO conversion of 93%at 160℃.Even under conditions of 8%(vol)H_(2)O and 0.016%(vol)SO_(2)(GHSV=300000 ml·h^(-1)·g^(-1)),the CO conversion remained above 95%at 220℃for 46 h.The catalysts were characterized and analyzed using various techniques.The results indicated that anatasephase TiO_(2) exhibited weak CO adsorption capacity but strong SO_(2) adsorption capacity,whereas rutilephase TiO_(2) demonstrated strong CO adsorption capacity and weak SO_(2) adsorption capacity.The presence of the anatase phase mitigated the CO self-poisoning phenomenon of the catalyst,while the biphase interface reduced the adsorption and oxidation of SO_(2) on the catalyst's surface,significantly inhibiting the deposition of TiOSO_4.Consequently,the Pt/TiO_(2)-500 catalyst displayed the highest CO catalytic activity along with superior resistance to sulfur and water.展开更多
文摘催化氧化技术是治理挥发性有机物(VOCs)的有效手段,其中新型催化剂的设计与优化是实现VOCs高效转化的关键。分别采用焙烧法与沉淀法制备了CeO_(2)活性载体,随后通过硼氢化钠还原法将Pt负载于CeO_(2)表面制备了Pt/CeO_(2)催化剂,进而考察了不同制备方法对其催化氧化甲苯性能的影响。通过XRD、N_(2)吸/脱附、紫外拉曼光谱、XPS及O_(2)-TPD等手段对催化剂进行了表征。通过in situ DRIFTS研究了甲苯在反应过程中的演变行为。结果表明,不同制备方法均调控了Pt/CeO_(2)催化剂中活性氧物种的浓度。其中,沉淀-还原法制备的Pt/CeO_(2)-P催化剂具有更高的活性氧物种和氧空位浓度,促进了甲苯的活化与转化,使其生成易于降解的甲酸盐物种,并最终氧化为CO_(2)和H_(2)O。在甲苯浓度(体积分数)为0.1%、空速为48000 m L/(g·h)条件下,Pt/CeO_(2)-P催化剂的T50和T90(甲苯转化率达到50%和90%时的反应温度)分别低至157℃和168℃。
基金supported by the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.ES202306).
文摘Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious metal ions,V_(2)O_(3)spiny hollow nanospheres(pV_(2)O_(3)SHN),was synthe sized through a one-step hydrothermal-as sis ted methodology for the adsorption of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) from the leaching solution of electronic waste.The results reveal that the p-V2O3SHN hierarchy was successfully constructed with a hollow structure and dense spiny morphology.The prepared p-V2O3SHN can effectively remove precious metal ions such as Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ),with the selective capture order being Au(Ⅲ)> Ag(Ⅰ)> Pt(Ⅳ)> Pd(Ⅱ)> other metal ions.This superior adsorption capability can be attributed to the multi-diffusible,intermingled composition,and numerous active sites decorating the p-V2O3SHN hierarchy,facilitating the uptake of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) ions from electronic waste.The Langmuir model provided a better fit for the uptake process,revealing maximum uptake capacities of 833.33 mg/g for Au(Ⅲ),370.37 mg/g for Ag(Ⅰ),42.01 mg/g for Pd(Ⅱ),and 77.51 mg/g for Pt(Ⅳ) on p-V_(2)O_(3)SHN.Remarkably,p-V_(2)O_(3)SHN exhibited a robust affinity for the adsorbate due to the presence of surface defects and reduction reactions.The new p-V2O3SHN also demonstrated good reusability for three sorption cycles,highlighting its potential for electronic waste treatment.Due to its facile synthesis and excellent efficiency,hierarchical p-V2O3SHN presents itself as a promising candidate for the selective uptake of Au(Ⅲ),Ag(Ⅰ),Pt(Ⅳ),and Pd(Ⅱ) from electronic waste.
基金supported by the National Natural Science Foundation of China(52002366,22075263,22571288)the Fundamental Research Funds for the Central Universities(WK2060000091,WK2060250115,WK2060000039)the Students’Innovation and Entrepreneurship Foundation of USTC(CY2023C021).
文摘The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batteries.To improve the reaction kinetics and decrease the reaction overpotential,we synthesized mesoporous Pt nanosheets with high tensile strain.The presence of many unsaturated coordinated Pt atoms around the pores gives rise to tensile strain in the mesoporous Pt nanosheets.This tensile strain plays a key role in regulating the interactions between the catalytic surface of Pt and the adsorbed intermediates.The two-dimensional structure provides more active sites on the surface for the catalytic reactions.These superiorities enable a low overpotential of 0.36 V at a cutoff capacity of 100μAh·cm^(−2) at a current density of 10μA·cm^(−2) over more than 2000 h.This study opens new possibilities for the rational design of metal-based materials with strain engineering for electrochemical energy storage.
基金financially supported by the National Key Research&Development Program of China(2024YFC3908400)the National Natural Science Foundation of China(U21B2099)Fundamental Research Funds for the Central Universities,Ocean University of China(202364004)。
文摘Catalytic oxidation is an effective strategy for eliminating CO pollutant.Pt/TiO_(2) catalyst are one of the most active catalysts as used,but facing the issue of sulfur and water deactivation.In this study,TiO_(2) was synthesized using a sol-gel method,while Pt/TiO_(2) was prepared by impregnation method.By varying the calcination temperature of the TiO_(2) support,Pt/TiO_(2) catalysts with different proportions of anatase and rutile phases were synthesized.At the calcination temperature of 500℃,the catalysts exhibited approximately equal proportions of anatase and rutile,resulting in exceptional catalytic activity for CO oxidation,as well as improved resistance to sulfur and water in the flue gas.Consequently,the Pt/TiO_(2)-500 catalyst achieved a CO conversion of 93%at 160℃.Even under conditions of 8%(vol)H_(2)O and 0.016%(vol)SO_(2)(GHSV=300000 ml·h^(-1)·g^(-1)),the CO conversion remained above 95%at 220℃for 46 h.The catalysts were characterized and analyzed using various techniques.The results indicated that anatasephase TiO_(2) exhibited weak CO adsorption capacity but strong SO_(2) adsorption capacity,whereas rutilephase TiO_(2) demonstrated strong CO adsorption capacity and weak SO_(2) adsorption capacity.The presence of the anatase phase mitigated the CO self-poisoning phenomenon of the catalyst,while the biphase interface reduced the adsorption and oxidation of SO_(2) on the catalyst's surface,significantly inhibiting the deposition of TiOSO_4.Consequently,the Pt/TiO_(2)-500 catalyst displayed the highest CO catalytic activity along with superior resistance to sulfur and water.
