The structural evolution and gasification reactivity of biochar prepared from the pyrolysis of wheat straw were investigated by in-situ Raman spectroscopy and thermogravimetric analysis.The Raman spectra consisted of ...The structural evolution and gasification reactivity of biochar prepared from the pyrolysis of wheat straw were investigated by in-situ Raman spectroscopy and thermogravimetric analysis.The Raman spectra consisted of a combination of four Lorentzian bands(D1,D2,D4,G)and one Gaussian band(D3)in the first-order region.The experimental results showed that the addition of catalysts or the presence of ash could improve the CO_(2) gasification reactivity of biochar and result in a larger ID1/IG ratio and a lower IG/IALL ratio,meaning that the carbon structure was less ordered,and there were also more active sites such as amorphous carbon and cross-linked structures;Ca-based catalysts and K-based catalysts changed the evolution of biochar structure in a different way in CO_(2) atmosphere,the ID3/ID1 of Ca-based biochar was close to the value of non-catalyst biochar and decreased slowly,indicating that the Ca-based catalysts can stabilize the aromatic rings,while the IG/IALL of K-based biochar decreases significantly and the ID3/ID1 increased significantly,indicating the increase of carbon structure defects and the cracking of large aromatic rings in bio-char into small ones;a scheme of K and Ca reaction with biochar in CO_(2) gasification process was proposed.展开更多
The effects of Mg,La and Ca promoters on primary and secondary CO2 and H2O formation pathways during Fischer-Tropsch synthesis on precipitated Fe/Cu/SiO2 catalysts are investigated.The chemisorbed oxygen atoms in the ...The effects of Mg,La and Ca promoters on primary and secondary CO2 and H2O formation pathways during Fischer-Tropsch synthesis on precipitated Fe/Cu/SiO2 catalysts are investigated.The chemisorbed oxygen atoms in the primary pathway formed in the CO dissociation steps reacted with co-adsorbed hydrogen or carbon monoxide to produce H2O and CO2,respectively.The secondary pathway was the water-gas shift reaction.The results indicated that the CO2 production led to an increase in both primary and secondary pathways,and H2O production decreased when surface basicity of the catalyst increased in the order Ca 〉 Mg 〉 La.展开更多
以植酸钙(PA-Ca)为载体、H2Pd Cl4为前驱体、甲醇为还原剂,制备了PA-Ca负载Pd的Pd/PA-Ca催化剂,对其进行XRF、BET、SEM、TEM、XRD和XPS表征,并用于苯甲醛氧化制备苯甲酸反应,考察催化剂用量、反应温度和溶剂种类对催化剂催化性能的影响...以植酸钙(PA-Ca)为载体、H2Pd Cl4为前驱体、甲醇为还原剂,制备了PA-Ca负载Pd的Pd/PA-Ca催化剂,对其进行XRF、BET、SEM、TEM、XRD和XPS表征,并用于苯甲醛氧化制备苯甲酸反应,考察催化剂用量、反应温度和溶剂种类对催化剂催化性能的影响。结果表明,催化剂中负载Pd质量分数为1.03%,钠质量分数为1.05%;合成的PA-Ca载体为晶化程度较低的介孔材料,比表面积为18.85 m^2·g^(-1);催化剂活性物种为Pd0和PdO。在催化剂用量n(苯甲醛)∶n(Pd)=2 000∶1、乙腈作溶剂、O_2压力101.325 k Pa(流速20 m L·min^(-1))、反应温度30℃和反应时间4 h条件下,苯甲醛转化率为83%,苯甲酸选择性为100%;催化剂具有较好的稳定性,可循环使用3~4次。展开更多
基金supported by the Shanghai Engineering Research Center of Coal Gasification(18DZ2283900)the Fundamental Research Funds for the Central Universities and the National Natural Science Foundation of China(21676091).
文摘The structural evolution and gasification reactivity of biochar prepared from the pyrolysis of wheat straw were investigated by in-situ Raman spectroscopy and thermogravimetric analysis.The Raman spectra consisted of a combination of four Lorentzian bands(D1,D2,D4,G)and one Gaussian band(D3)in the first-order region.The experimental results showed that the addition of catalysts or the presence of ash could improve the CO_(2) gasification reactivity of biochar and result in a larger ID1/IG ratio and a lower IG/IALL ratio,meaning that the carbon structure was less ordered,and there were also more active sites such as amorphous carbon and cross-linked structures;Ca-based catalysts and K-based catalysts changed the evolution of biochar structure in a different way in CO_(2) atmosphere,the ID3/ID1 of Ca-based biochar was close to the value of non-catalyst biochar and decreased slowly,indicating that the Ca-based catalysts can stabilize the aromatic rings,while the IG/IALL of K-based biochar decreases significantly and the ID3/ID1 increased significantly,indicating the increase of carbon structure defects and the cracking of large aromatic rings in bio-char into small ones;a scheme of K and Ca reaction with biochar in CO_(2) gasification process was proposed.
文摘The effects of Mg,La and Ca promoters on primary and secondary CO2 and H2O formation pathways during Fischer-Tropsch synthesis on precipitated Fe/Cu/SiO2 catalysts are investigated.The chemisorbed oxygen atoms in the primary pathway formed in the CO dissociation steps reacted with co-adsorbed hydrogen or carbon monoxide to produce H2O and CO2,respectively.The secondary pathway was the water-gas shift reaction.The results indicated that the CO2 production led to an increase in both primary and secondary pathways,and H2O production decreased when surface basicity of the catalyst increased in the order Ca 〉 Mg 〉 La.
文摘以植酸钙(PA-Ca)为载体、H2Pd Cl4为前驱体、甲醇为还原剂,制备了PA-Ca负载Pd的Pd/PA-Ca催化剂,对其进行XRF、BET、SEM、TEM、XRD和XPS表征,并用于苯甲醛氧化制备苯甲酸反应,考察催化剂用量、反应温度和溶剂种类对催化剂催化性能的影响。结果表明,催化剂中负载Pd质量分数为1.03%,钠质量分数为1.05%;合成的PA-Ca载体为晶化程度较低的介孔材料,比表面积为18.85 m^2·g^(-1);催化剂活性物种为Pd0和PdO。在催化剂用量n(苯甲醛)∶n(Pd)=2 000∶1、乙腈作溶剂、O_2压力101.325 k Pa(流速20 m L·min^(-1))、反应温度30℃和反应时间4 h条件下,苯甲醛转化率为83%,苯甲酸选择性为100%;催化剂具有较好的稳定性,可循环使用3~4次。
