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High-perf.rmance oxygen reduction and evolution carbon catalysis： f.om mechanistic studies to device integration

Nano Research 2017年第4期10卷 1163-1177页

作者： John W. f. To Jia Wei Desmond Ng Samira Siahrostami Ai Leen Koh Yangjin Lee Zhihua Chen Kara D. f.ng Shucheng Chen Jiajun He Won-Gyu Bae Jennif.r Wilcox Hu Young Jeong Kwanpyo Kim f.lix Studt Jens K. Nфrskov thomas f. jaramillo Zhenan Bao Department of.Chemical Engineering Stan ford University Stanford CA 94305 USA Institute of.Chemical and Engineering Sciences Agency for Science Technology and Research Jurong Island 627833 Singapore Stanf.rd Nano Shared f.cilities Stanford University Stanford CA 94305 USA Department of.Physics Ulsan National Institute of Science and Technology (UNIST) Ulsan 689-798 Republic of Korea Department of.Chemical and Biological Engineering Colorado School of Mines Golden CO 80401 USA UNIST Central Research f.cilities (UCRf. Ulsan National Institute of Science and Technology (UNIST) Ulsan 689-798 Republic of Korea SUNCAT Center f.r Interf.ce Science and Catalysis SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park CA 94025 USA Institute of.Catalysis Research and Technology Karlsruhe Institute of Technology Hermann-von-Helmholtz Platz 1 76344 Eggenstein-Leopoldshafen Germany Institute f.r Chemical Technology and Polymer Chemistry Karlsruhe Institute of Technology Engesserstr. 18 76131 Karlsruhe Germany

The development of.high-perf.rmance and low-cost oxygen reduction and evolution catalysts that can be easily integrated into existing devices is crucial f.r the wide deployment of.energy storage systems that utilize O2-H2O chemistries, such as regenerative f.el cells and metal-air batteries. Herein, we report an NHB-activated N-doped hierarchical carbon （NHC） catalyst synthesized via a scalable route, and demonstrate its device integration. The NHC catalyst exhibited good perf.rmance f.r both the oxygen reduction reaction （ORR） and the oxygen evolution reaction （OER）, as demonstrated by means of.electrochemical studies and evaluation when integrated into the oxygen electrode of.a regenerative f.el cell. The activities observed f.r both the ORR and the OER were comparable to those achieved by state-of.the-art Pt and Ir catalysts in alkaline environments. We have f.rther identif.ed the critical role of.carbon def.cts as active sites f.r electrochemical activity through density f.nctional theory calculations and high-resolution TEM visualization. This work highlights the potential of.NHC to replace commercial precious metals in regenerative f.el cells and possibly metal-air batteries f.r cost-ef.ective storage of.intermittent renewable energy.

关键词： electrocatalysis porous carbon density f.nctional theory

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Carbon f.owers as electrocatalysts f.r the reduction of.oxygen to hydrogen peroxide

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Nano Research 2023年第9期16卷 11556-11563页

作者： Huaxin Gong Lingze Wei Shucheng Chen Zhihua Chen thomas f.jaramillo Zhenan Bao Department of.Chemical Engineering Stanford UniversityStanfordCA 94305USA SUNCAT Center f.r Interf.ce Science and Catalysis SLAC National Accelerator LaboratoryMenlo ParkCA 94025USA

Small-scale and decentralized production of.H_(2)O_(2)via electrochemical reduction of.oxygen is of.great benef.t,especially f.r sanitization,air and water purif.cation,as well as f.r a variety of.chemical *** development of.low-cost and highperf.rmance catalysts f.r this reaction remains a key ***-based materials have drawn substantial research ef.orts in recent years due to their advantageous properties,such as high chemical stability and high tunability in active sites and *** understanding of.structure–activity relationships can guide the design of.improved *** hypothesize that mass transport to active sites is of.great importance,and herein we use carbon materials with unique f.ower-like superstructures to achieve high activity and selectivity f.r O2 reduction to H_(2)O_(2).The abundance of.nitrogen active sites controlled by pyrolysis temperature resulted in high catalytic activity and selectivity f.r oxygen reduction reaction(ORR).The f.ower superstructure showed higher perf.rmance than the spherical nanoparticles due to greater accessibility to the active *** activation improves the catalysts’perf.rmances f.rther,driving the production of.H_(2)O_(2)to a record-setting rate of.816 mmol·gcat^(−1)·h^(−1)using a bulk electrolysis *** work demonstrates the development of.a highly active catalyst f.r the sustainable production of.H_(2)O_(2)through rational design and synthetic *** understanding f.om this work provides f.rther insight into the design of.f.ture carbon-based electrocatalysts.

关键词： carbon materials H_(2)O_(2) oxygen reduction reaction nanostructures

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Towards predicting biochar impacts on plant-available soil nitrogen content

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Biochar 2022年第1期4卷 1040-1054页

作者： Claire L.Phillips Kylie M.Meyer Manuel Garcia-jaramillo Clara S.Weidman Catherine E.Stewart thomas Wanzek Michael A.Grusak Donald W.Watts Jef. Novak Kristin M.Trippe USDA-ARS National Laboratory f.r Agriculture and Environment AmesIAUSA USDA-ARS f.rage Seed and Cereal Research Unit CorvallisORUSA Department of.Environmental Toxicology Oregon State UniversityCorvallisORUSA Department of.Crop and Soil Science Oregon State UniversityCorvallisORUSA USDA-ARS Soil Management and Sugarbeet Research Unit Ft.CollinsCOUSA USDA-ARS Edward T.Schaf.r Agricultural Research Center FargoNDUSA USDA-ARS Coastal Plain Soil Waterand Plant Research CenterFlorenceSCUSA

Biochars can improve soil health but have been widely shown to reduce plant-available nitrogen(N)owing to their high carbon(C)content,which stimulates microbial ***,because biochars contain large amounts of.C that are not microbially available,their total elemental C:N ratio does not correspond well with impacts on soil *** hypothesized that impacts on soil plant-available N would relate to biochar mineralizable-C(C_(min))content,and that C:N ratios of.the mineralizable biochar component could provide a means f.r predicting conditions of.net soil N-mineralization *** conducted two laboratory experiments,the f.rst measuring biochar C_(min)f.om respiration of.isotopically labeled barley biochars manuf.ctured at 300,500,and 750℃,and the second characterizing C_(min)by proxy measurements f.r ten biochars f.om six f.edstocks at several *** both experiments,soils were incubated with 2%biochar by mass to determine impacts to soil *** to expectation,all the biochars increased soil N-mineralization relative to unamended *** unexpected,higher temperature(500 and 700℃)barley biochars with less C_(min)stimulated more soil decomposition and more soil N-mineralization than a 350℃barley ***,across diverse biochar f.edstocks and production methods,none of.the biochar characteristics correlated with soil *** f.nding of.improved soil N-mineralization adds complexity to the range of.soil N responses that can be expected in response to biochar *** of.the limited ability to predict soil N responses f.om biochar properties,users should monitor soil N to manage soil f.rtility.

关键词： C:N ratio Plant-available nitrogen Priming Respiration ^(13)C

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Tracing Water f.ow and Colloidal Particles Transf.r in an Unsaturated Soil

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Journal of.Water Resource and Protection 2014年第7期6卷 696-709页

作者： Dieuseul Prédélus Laurent Lassabatere Artur Paiva Coutinho Cédric Louis thomas Brichart Erij Ben Slimène Thierry Winiarski Raf.el Angulo-jaramillo Nano-H S.A.S. 38070 Saint Quentin Fallavier France Universidade f.deral de Pernambuco Recife Brazil Université de Lyon CNRS UMR 5023 LEHNA ENTPE Vaulx-en-Velin France Universidade f.deral de Pernambuco Recife Brazil

In recent years, many studies have been carried out on colloidal particle transf.r in the unsaturated zone because they can be a risk to the environment either directly or as a vector of.pollutants. A study was conducted on the inf.uence of.porous media structure in unsaturated conditions on colloidal particle transport. Three granular materials were set up in columns to replicate a f.uvio-glacial soil f.om the unsaturated zone in the Lyon area (f.ance). It is a sand, a bimodal mixture in equal proportion by weight of.sand and gravel, and a f.action of.bimodal mixture. Nanoparticles of.silica (SiO2-Au-f.uoNPs), having a hydrodynamic diameter between 50 and 60 nm, labeled by organic f.uorescent molecules were used to simulate the transport of.colloidal particles. A nonreactive tracer, bromide ion (Br-) at a concentration of.C0,s = 10-2 M was used to determine the hydrodispersive properties of.porous media. The tests were carried out f.rst, with a solution of.nanoparticles (C0,p = 0.2 g/L) and secondly, with a solution of.nanoparticles and bromine. The transf.r model based on f.actionation of.water into two phases, mobile and immobile, MIM, correctly f.ts the elution curves. The retention of.colloidal particles is greater in the two media of.bimodal particle size than that in the sand, which clearly demonstrates the role of.textural heterogeneity in the retention mechanism. The increase in ionic strength produced by alimenting the columns with colloidal particle suspension in the presence of.bromide, increases retention up to 25% in the sand. The total concentration prof.le of.nanoparticles collected at the end of.the experiment shows that the colloidal particles are retained primarily at the entrance of.the columns. Hydrodispersive calculated parameters indicate that f.ow is more heterogeneous in bimodal media compared to sand.

关键词： Colloidal Particle Transport Microstructure Modeling Unsaturated Soil

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