The electrochemical conversion of CO₂ into liquid fuels offers alternative ways to produce renewable fuels and store the surplus renewable energy. However, significant chemistry challenges still remain, particularly in relation to the kinetic inertness of CO₂ and thermodynamic complexity of the multiple electron transfer processes involved. We describe a new type of flow-Through membrane reactor, based on a hierarchically ordered platinum nanochannel array with macropore channels in combination with mesoporous walls. The membrane reactor exhibits unique three-dimensional electrocatalytic interfaces with high activity and selectivity in CO₂ conversion producing methanol and ethanol as the dominant liquid products. The Faradaic efficiency and yield for alcohol production are up to 23.9% and 2.1 × 10^-8 mol s^-1 cm^-2 at 51 mA/cm^-2, respectively. Experimental and density functional theory studies evidence that substantial (110) facets and a high density of atomic surface steps contribute significantly to the intrinsic activity and selectivity for conversion of CO₂ to alcohol.

Xinyi Zhang;Bingmei Huang;Chenghua Sun;威 卢;Zhi Qun Tian;培康 沈;Huanting Wang;东元 赵;Douglas R. Macfarlane

ACS Energy Letters

2018-11-9

Three-dimensional (3D) cubic ordered macroporous (140 nm) and binary macroporous (140, 80 nm) silica structures with ordered mesoporous (7.7 nm) walls have been synthesized by using cubic closed-packing colloidal crystals as templates. The colloidal crystals can be made from equal-sized or binary-sized latex spheres by the simple methods of self-sedimentation on the film or pressing into a pellet.

Qian Luo;Li Li;柏 杨;东元 赵

Chemistry Letters

2000

A strategy of protein entrapment within mesoporous carbon matrices is demonstrated to probe the electrochemistry of glucose oxidase. Large surface area and remarkable electro-catalytic properties of carbon mesoporous materials make them suitable candidates for high loading of protein molecules and the promotion of heterogeneous electron transfer. In this work, two kinds of mesoporous carbon nanocomposite films were designed and prepared with highly ordered two-dimensional (2D) and three-dimensional (3D) structures for the immobilization of glucose oxidase, in which the quasi-reversible electron transfer of the redox enzyme was probed, and the apparent heterogeneous electron transfer rate constants (k_et ⁰) are 3.9 and 4.2 s^-1, respectively. Furthermore, the associated biocatalytic activity was also revealed. Highly ordered 3D-mesoporous carbon material exhibited larger adsorption capacity for glucose oxidase and the immobilized enzymes retained a higher bioactivity compared with 2D-mesoporous carbons. The preparation of protein-entrapped mesoporous carbon nanocomposites expands the scope of carbon-based electrochemical devices and opens a new avenue for the development of biosensors.

Chunping You;昕 徐;Bozhi Tian;继烈 孔;东元 赵;宝红 刘

Talanta

2009-5-15

Hierarchically ordered macro-/mesoporous TiO₂ films with a large surface area, huge pore volume, highly crystalline framework, and continuous morphology are successfully synthesized using a confined evaporation-induced self-assembly (EISA) method accompanied by a surfactant sulfuric acid carbonization method. The films exhibit excellent photoelectrocatalytic water-splitting performance.

Renyuan Zhang;Dengke Shen;Ming Xu;Dan Feng;Wei Li;耿锋 郑;仁超 车;Ahmed A. Elzatahry;东元 赵

Advanced Energy Materials

2014-6-3

A new microporous zirconogermanate, diammonium zirconium trigermanate, (NH₄)₂ZrGe₃O₉ (FDZG-2), analogous to wadeite (K₂ZrSi₃O₉), was hydrothermally synthesized using ZrO(NO₃)₂·2H₂O as the source of zirconium and 1,4-diaminobutane as a structure-directing agent. Single-crystal X-ray diffraction analysis reveals that the framework structure is built up of cyclic trigermanate units crosslinked by ZrO₆ octahedra. The Zr atom lies at a site with 3̄ symmetry and the unique N atom of the ammonium ion lies at a site with threefold symmetry. Large cages are observed, with two NH₄⁺ cations in each. The structure contains intersecting six- and three-membered ring (6MR and 3MR) channels, but only the 6MR channels can accommodate the NH₄⁺ ions.

Zhicheng Liu;Linhong Weng;Zhenxia Chen;东元 赵

Acta Crystallographica Section C: Crystal Structure Communications

2003-5

Well ordered, uniform 3D open macro/mesoporous TiO₂ hollow microspheres with highly crystalline anatase thin shells have been successfully synthesized by a simple solvent evaporation-driven confined self-assembly method. The 3D open macro/mesoporous TiO₂ hollow microspheres show high energy-conversion efficiency (up to 9.5%) and remarkable photocatalytic activity (with photodegradation of 100% for methylene blue in 12 min under UV light irradiation).

Yong Liu;Kun Lan;Abdulaziz A. Bagabas;Pengfei Zhang;Wenjun Gao;Jingxiu Wang;Zhenkun Sun;Jianwei Fan;Ahmed A. Elzatahry;东元 赵

Small

2016-2-17

Rational design and controllable synthesis of TiO₂ based materials with unique microstructure, high reactivity, and excellent electrochemical performance for lithium ion batteries are crucially desired. In this paper, we developed a versatile route to synthesize hollow TiO₂/graphitic carbon (H-TiO₂/GC) spheres with superior electrochemical performance. The as-prepared mesoporous H-TiO₂/GC hollow spheres present a high specific surface area (298 m² g^-1), a high pore volume (0.31 cm³ g^-1), a large pore size (∼5 nm), well-defined hollow structure (monodispersed size of 600 nm and inner diameter of ∼400 nm, shell thickness of 100 nm), and small nanocrystals of anatase TiO₂ (∼8 nm) conformably encapsulated in ultrathin graphitic carbon layers. As a result, the H-TiO₂/GC hollow spheres achieve excellent electrochemical reactivity and stability as an anode material for lithium ion batteries. A high specific capacity of 137 mAh g^-1 can be achieved up to 1000 cycles at a current density of 1 A g^-1 (5 C). We believe that the mesoporous H-TiO₂/GC hollow spheres are expected to be applied as a high-performance electrode material for next generation lithium ion batteries.

Hao Liu;Wei Li;Dengke Shen;东元 赵;Guoxiu Wang

Journal of the American Chemical Society

2015-10-14

Monodisperse mesoporous silica microparticles (50 to 100 μm) can be produced via a microfluidic jet spray-drying route, using cetyl trimethylammonium bromide (CTAB) or pluronic F127 as templating agents, and tetraethylorthosilicate (TEOS) for silica. The microparticles demonstrate highly ordered hexagonal mesostructures with surface areas from ~ 900 up to 1500 m²/g and pore volumes from ~ 0.6 to 0.8 cm³/g. Here, the spray drying of dual surfactant-templated silica, and dual-surfactant templated carbon-silica composites are presented, with discussion on the possible interactions governing meso- and macro-structure formations and the hierarchical structures formed through evaporation-induced self assembly via spray drying.

K. Waldron;Z. Wu;东元 赵;X. D. Chen;C. Selomulya

Materials Today: Proceedings

2016

Patrick Schmidt-Winkel;Wayne W. Lukens;东元 赵;Peidong Yang;Bradley F. Chmelka;Galen D. Stucky

Journal of the American Chemical Society

1999-1-13

To alleviate the environmental and health threats from water resources polluted by large-sized microcystins (MCs), we demonstrate for the first time that ordered mesoporous silica materials with large pore sizes of 2-12 nm can be used as adsorbents for rapid and efficient removal of MCs. The obvious correlations between adsorption performance of MCs and physicochemical properties of adsorbents including pore mesostructure, texture and size, and surface chemistry have been well established. Accordingly, an excellent candidate, mesoporous silica SBA-15 templated from Pluronic P123 has been sorted out, exhibiting extremely rapid rate (one minute) as well as high capacities of 5.99 and 13 mg g^-1 for removing high-concentration MC-LR and MC-RR, respectively, which are much higher than that of other silica-based adsorbents reported previously. The adsorption performance can be further improved from 50 to 95% at around pH 4 by grafting positively charged and/or hydrophobic groups onto pore surface of SBA-15. Furthermore, thermodynamic and kinetic evaluations provide additional valuable information for a better understanding of the adsorption process. Given the excellent adsorption performance, it is expected that mesoporous silica materials with unique characteristics are attractive for actual applications in removal of MCs from wastewater.

Wei Teng;Zhangxiong Wu;Dan Feng;Jianwei Fan;Jinxiu Wang;Hao Wei;Mingjuan Song;东元 赵

Environmental Science & Technology

2013-8-6