Hydrogenation of lignin-derived phenol to KA oil(the mixture of cyclohexanone(K)and cyclohexanol(A))is attractive yet challenging in the sustainable upgrading of biomass derivatives under mild conditions.Traditional s...Hydrogenation of lignin-derived phenol to KA oil(the mixture of cyclohexanone(K)and cyclohexanol(A))is attractive yet challenging in the sustainable upgrading of biomass derivatives under mild conditions.Traditional supported metal catalysts have been widely studied but the active components on supports often exhibit low recyclability due to their instability under experimental conditions.Here we show fabricating ultrasmall Pt/NiO in the pores of chromium terephthalate MIL-101 as catalysts for hydrogenation of phenol.Impressively,Pt/NiO@MIL-101 achieves catalytic phenol hydrogenation to KA oils of tunable K/A ratios and good reusability under room temperature and atmospheric hydrogen pressure,superior to contrast Pt@MIL-101 and Pt/NiO samples.Such excellent performance mainly originates from the effective adsorption and activation of phenol by coordinatively unsaturated Cr sites and H2 activation on ultrasmall Pt/NiO as well as its effective spillover to the adsorbed phenol over Cr sites for hydrogenation reaction.Substantially,such catalyst also displays the excellent performances for hydrogenation of phenol’s derivatives under mild conditions.展开更多
以硝酸镍为镍源,通过水热法制成NiO-C载体,随后利用L-抗坏血酸和氢气将铂离子镶嵌入载体中,制备出Pt和NiO共存的Pt@NiO-C催化剂,并对其全解水性能进行测试。首先运用XRD、SEM、XPS等测试手段,对材料组成与结构进行了表征。结果表明,半导...以硝酸镍为镍源,通过水热法制成NiO-C载体,随后利用L-抗坏血酸和氢气将铂离子镶嵌入载体中,制备出Pt和NiO共存的Pt@NiO-C催化剂,并对其全解水性能进行测试。首先运用XRD、SEM、XPS等测试手段,对材料组成与结构进行了表征。结果表明,半导体NiO不仅可以作为析氢贵金属载体,同时也可以为析氧提供活性点位。电化学测试结果显示,在浓度为0.5 mol/L的硫酸溶液中,Pt@NiO-C材料的析氢起始电位仅为25 mV(VS.RHE),塔菲尔斜率为31 m V·dec^(-1),经过20个小时的连续工作依旧能保持稳定的催化性能,析氧性能优于商用铂碳(20%),为质子交换膜制氢技术的发展提供一种新的思路。展开更多
基金the National Key Research and Development Program of China(No.2021YFA1500403)Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)+1 种基金the National Natural Science Foundation of China(Nos.52372079,22173024,and 21722102)Youth Innovation Promotion Association CAS(G.D.L.).
文摘Hydrogenation of lignin-derived phenol to KA oil(the mixture of cyclohexanone(K)and cyclohexanol(A))is attractive yet challenging in the sustainable upgrading of biomass derivatives under mild conditions.Traditional supported metal catalysts have been widely studied but the active components on supports often exhibit low recyclability due to their instability under experimental conditions.Here we show fabricating ultrasmall Pt/NiO in the pores of chromium terephthalate MIL-101 as catalysts for hydrogenation of phenol.Impressively,Pt/NiO@MIL-101 achieves catalytic phenol hydrogenation to KA oils of tunable K/A ratios and good reusability under room temperature and atmospheric hydrogen pressure,superior to contrast Pt@MIL-101 and Pt/NiO samples.Such excellent performance mainly originates from the effective adsorption and activation of phenol by coordinatively unsaturated Cr sites and H2 activation on ultrasmall Pt/NiO as well as its effective spillover to the adsorbed phenol over Cr sites for hydrogenation reaction.Substantially,such catalyst also displays the excellent performances for hydrogenation of phenol’s derivatives under mild conditions.
文摘以硝酸镍为镍源,通过水热法制成NiO-C载体,随后利用L-抗坏血酸和氢气将铂离子镶嵌入载体中,制备出Pt和NiO共存的Pt@NiO-C催化剂,并对其全解水性能进行测试。首先运用XRD、SEM、XPS等测试手段,对材料组成与结构进行了表征。结果表明,半导体NiO不仅可以作为析氢贵金属载体,同时也可以为析氧提供活性点位。电化学测试结果显示,在浓度为0.5 mol/L的硫酸溶液中,Pt@NiO-C材料的析氢起始电位仅为25 mV(VS.RHE),塔菲尔斜率为31 m V·dec^(-1),经过20个小时的连续工作依旧能保持稳定的催化性能,析氧性能优于商用铂碳(20%),为质子交换膜制氢技术的发展提供一种新的思路。
