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| 1 | 调变锌基水滑石三价/四价金属实现高选择性光催化CO2还原显示文摘光催化CO2还原是一项生产燃料和化学品的未来技术,然而至今影响还原产物选择性的因素仍然不甚清楚.本文对比了一系列锌基水滑石(ZnM-LDH)光催化材料的CO2还原性能,通过改变ZnM LDH中三价或四价金属离子组成,可以精确控制反应产物的选择性.其中ZnTi-LDH以甲烷为主要还原产物,ZnFe-LDH和ZnCo-LDH仅能通过光催化水分解反应生成氢气,而ZnGa-LDH和ZnAl-LDH的主要产物是一氧化碳.采用原位漫反射红外光谱、价带X射线光电子能谱和密度函数理论计算,对影响ZnM-LDH光催化CO2还原选择性的因素进行了详细讨论.结果表明,M3+或M4+离子的d带中心位置是影响CO2吸附强度的主要因素,从而控制了对含碳产物或氢气的选择性.本文的发现阐明了三价和四价金属离子在水滑石光催化材料中调控CO2还原产物选择性的作用,为开发具有高指定产物选择性的水滑石光催化材料开辟了新途径. | 熊旭阳 赵宇飞 施润 殷文金 赵运宣 Geoffrey INWaterhouse 张铁锐 | 2020 | Science Bulletin2020，65，12： | 12 |
| 2 | Highly Efficient Photoelectrocatalytic Reduction of CO2 to Methanol by a p–n Heterojunction CeO2/CuO/Cu Catalyst显示文摘Photoelectrocatalytic reduction of CO2 to fuels has great potential for reducing anthropogenic CO2 emissions and also lessening our dependence on fossil fuel energy.Herein,we report the successful development of a novel photoelectrocatalytic catalyst for the selective reduction of CO2 to methanol,comprising a copper catalyst modified with flower-like cerium oxide nanoparticles(CeO2 NPs)(a n-type semiconductor)and copper oxide nanoparticles(CuO NPs)(a p-type semiconductor).At an applied potential of−1.0 V(vs SCE)under visible light irradiation,the CeO2 NPs/CuO NPs/Cu catalyst yielded methanol at a rate of 3.44μmol cm^−2 h^−1,which was approximately five times higher than that of a CuO NPs/Cu catalyst(0.67μmol cm^−2 h^−1).The carrier concentration increased by^108 times when the flower-like CeO2 NPs were deposited on the CuO NPs/Cu catalyst,due to synergistic transfer of photoexcited electrons from the conduction band of CuO to that of CeO2,which enhanced both photocatalytic and photoelectrocatalytic CO2 reduction on the CeO2 NPs.The facile migration of photoexcited electrons and holes across the p–n heterojunction that formed between the CeO2 and CuO components was thus critical to excellent light-induced CO2 reduction properties of the CeO2 NPs/CuO NPs/Cu catalyst.Results encourage the wider application of composite semiconductor electrodes in carbon dioxide reduction. | Zhengbin Pan Ershuan Han Jingui Zheng Jing Lu Xiaolin Wang Yanbin Yin Geoffrey INWaterhouse Xiuguo Wang Peiqiang Li | 2020 | Nano-Micro Letters2020，12，2： | 3 |
| 3 | 碳点衍生的碳纳米花负载钴单原子和纳米颗粒用于高效的氧还原反应显示文摘锌空气电池(ZABs)具有高能量密度(1086 mWh gZn^(–1))、价低、易回收等优势,引起了学者们的广泛关注.空气电极发生的氧还原反应(ORR)/氧析出反应(OER)是控制整个ZABs效率的关键.因此,设计和开发高效的ORR电催化剂对于ZABs商业化至关重要.目前,Pt基电催化剂仍是最有效的ORR电催化剂,但Pt资源稀缺,价格高昂,Pt基电催化剂稳定性差等缺点阻碍了其商业化.因此,研究高活性和高稳定性的ORR非贵金属电催化剂十分重要.碳点(CDs)作为一种新型的零维高分子碳材料,具有低毒、高导电性等优势,被广泛用于碳基材料的前驱体.CDs具有sp^(2)杂化晶核、丰富的边缘位点和大量的官能团(如‒NH_(2),‒COOH和‒OH),这些表面官能团为过渡金属原子提供了很强的锚定位点,可用于构筑各种碳负载过渡金属催化剂.本文设计合成了一种新型的碳基ORR电催化剂,其由CDs衍生的三维碳纳米花(CNF)负载Co单原子(SAs)和纳米颗粒(NPs)构成.利用CDs在二次水热过程中形成了3.66 nm的超薄纳米膜并构筑成3D的多孔CNF结构.X射线衍射、高角度环形暗场原子分辨率扫描跃迁电子显微镜和X射线吸收光谱结果表明,材料中的SAs和NPs共存.测试结果表明,Co SAs/NPs CNF拥有可以和商业Pt/C相当的ORR活性(E_(1/2)=0.83 V(vs.RHE),j_(L)=6.13 mA cm^(-2)),且具有良好的稳定性.同时,利用SCN–可以毒化SAs和NPs,而EDTA只能毒化SAs的特性,证明了Co SAs和Co NPs协同促进了整个催化反应过程.理论计算表明,相邻Co NPs的存在优化了Co-N_(4)位点的电子结构,显著降低了ORR决速步骤(*OOH吸附)的能垒.因此,在整个催化反应过程中,Co SAs和Co NPs协同改善了ORR过程中的电子和质子转移行为.Co SAs/NPs CNF较大的比表面积和丰富的多孔结构有利于O_(2)和质子传输,基于其组装的ZABs的能量密度高达1000.58 mWh gZn^(–1)(理论值的93.69%)和循环运行1300次性能依然稳定.综上,本工作为高性能ORR电催化剂的设计提供依据. | 程瑶佳 宋昊强 于镜坤 常江伟 Geoffrey INWaterhouse 唐智勇 杨柏 卢思宇 | 2022 | Chinese Journal of Catalysis2022，43，9： | 1 |
| 4 | Pectin fractions extracted sequentially from Cerasus humilis:Their compositions,structures,functional properties and antioxidant activities显示文摘Three pectin fractions(water-soluble fraction(WSF),chelator-soluble fraction(CSF),and sodium carbonatesoluble fraction(NSF))were obtained from Chinese dwarf cherry(Cerasus humilis)fruits.All of them were branched low methoxylated pectins with an amorphous or partially nanocrystalline nature and eight neutral monosaccharides(arabinose and galactose were most abundant).WSF,CSF and NSF had a degree of methylation(DM)of 35.82%,14.85%and 7.13%,uronic acid(UA)content of 76.02%,83.71%and 69.01%,and total protein content of 2.4%,2.1%and 8.8%,respectively.Their molecular weights were 340.31,330.16 and 141.31 kg/mol,respectively(analyzed by gel permeation chromatography(GPC)).WSF,CSF and NSF exhibited good rheological,thermal,emulsifying,emulsion-stabilizing,water-adsorbing,oil-binding,cholesterol-binding and antioxidant properties.NSF had the highest emulsifying,emulsion stabilizing,water-/oil-/cholesterol-binding and antioxidant capacities,followed by CSF.NSF had the highest viscosity(406.77 m Pa·s),flowability,and resistance to heat-induced changes/damage,which may be related to its lowest polydispersity index,DM and UA content and highest protein content.The three pectin fractions with desirable characteristics can be used as food additives/ingredients and dietary supplements. | Shikai Zhang Geoffrey INWaterhouse Tingting Cui Dongxiao Sun-Waterhouse Peng Wu | 2023 | Food Science and Human Wellness2023，12，2： | 0 |
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