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Hierarchically porous cellulose nanofibril aerogel decorated with polypyrrole and nickel-cobalt layereddouble hydroxide for high-performance nonenzymatic glucose sensors

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1593-1607 doi: 10.1007/s11705-023-2348-2

摘要: With increasing emphasis on green chemistry, biomass-based materials have attracted increased attention regarding the development of highly efficient functional materials. Herein, a new pore-rich cellulose nanofibril aerogel is utilized as a substrate to integrate highly conductive polypyrrole and active nanoflower-like nickel-cobalt layered double hydroxide through in situ chemical polymerization and electrodeposition. This ternary composite can act as an effective self-supported electrode for the electrocatalytic oxidation of glucose. With the synergistic effect of three heterogeneous components, the electrode achieves outstanding glucose sensing performance, including a high sensitivity (851.4 µA·mmol−1·L·cm−2), a short response time (2.2 s), a wide linear range (two stages: 0.001−8.145 and 8.145−35.500 mmol·L−1), strong immunity to interference, outstanding intraelectrode and interelectrode reproducibility, a favorable toxicity resistance (Cl), and a good long-term stability (maintaining 86.0% of the original value after 30 d). These data are superior to those of some traditional glucose sensors using nonbiomass substrates. When determining the blood glucose level of a human serum, this electrode realizes a high recovery rate of 97.07%–98.89%, validating the potential for high-performance blood glucose sensing.

关键词: cellulose nanofibril     aerogel     nickel-cobalt layered double hydroxide     polypyrrole     nonenzymatic glucose sensor    

Defective Nickle–Iron Layered Double Hydroxide for Enhanced Photocatalytic NO Oxidation with Significant

Xiaoyu Li,Xiaoshu Lv,Jian Pan,Peng Chen,Huihui Peng,Yan Jiang,Haifeng Gong,Guangming Jiang,Li'an Hou,

《工程(英文)》 doi: 10.1016/j.eng.2023.06.017

摘要: Photocatalysis offers a sustainable avenue for the oxidative removal of low concentrations of NOx from the atmosphere. Layered double hydroxides (LDHs) are promising candidate photocatalysts owing to their unique layered and tunable chemical structures, and the abundant hydroxide (OH−) moieties on their surfaces that are hydroxyl radical (•OH) precursors. However, inferior charge separation and limited active sites on an LDH hinder its practical applications. Herein, we developed a facile N2H4-driven etching (et) approach that introduces dual Ni2+ and OH− vacancies (Niv and OHv) into NiFe-LDH nanosheets (referred to as NiFe-LDH-et) that facilitate improved charge-carrier separation and the formation of active Lewis acidic sites (Fe3+ and Ni2+ exposed at OHv). In contrast to inert pristine LDH, NiFe-LDH-et actively removes NO when illuminated with visible light. Specifically, Ni76Fe24-LDH-et etched in 1.50 mmol·L−1 N2H4 solution removes 32.8% of the NO from continuously flowing air (NO-feed concentration: ∼500 parts per billion (ppb)) when illuminated with visible light, thereby outperforming most reported catalysts. Experimental and theoretical data reveal that the dual vacancies promote the production of reactive oxygen species (•O2− and •OH) and the adsorption of NO on the LDH. In-situ spectroscopy revealed that NO is preferentially adsorbed at Lewis acidic sites, particularly exposed Fe3+ sites, and then converted into NO+ that is subsequently oxidized to NO3− without the formation of any of the more toxic NO2 intermediate, thereby alleviating risks associated with its production and emission.

关键词: Vacancies     Layered double hydroxide     NO     +     Photocatalysis     NO removal    

Layered double hydroxide-based core-shell nanoarrays for efficient electrochemical water splitting

Wenfu Xie, Zhenhua Li, Mingfei Shao, Min Wei

《化学科学与工程前沿(英文)》 2018年 第12卷 第3期   页码 537-554 doi: 10.1007/s11705-018-1719-6

摘要:

Electrochemical water splitting is an efficient and clean strategy to produce sustainable energy productions (especially hydrogen) from earth-abundant water. Recently, layered double hydroxide (LDH)-based materials have gained increasing attentions as promising electrocatalysts for water splitting. Designing LDHs into hierarchical architectures (e.g., core-shell nanoarrays) is one of the most promising strategies to improve their electrocatalytic performances, owing to the abundant exposure of active sites. This review mainly focuses on recent progress on the synthesis of hierarchical LDH-based core-shell nanoarrays as high performance electrocatalysts for electrochemical water splitting. By classifying different nanostructured materials combined with LDHs, a number of LDH-based core-shell nanoarrays have been developed and their synthesis strategies, structural characters and electrochemical performances are rationally described. Moreover, further developments and challenges in developing promising electrocatalysts based on hierarchical nanostructured LDHs are covered from the viewpoint of fundamental research and practical applications.

关键词: layered double hydroxides (LDHs)     core-shell nanoarrays     oxygen evolution reaction (OER)     hydrogen evolution reaction (HER)     photoelectrochemical water splitting (PEC)    

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

《化学科学与工程前沿(英文)》 2017年 第11卷 第4期   页码 613-623 doi: 10.1007/s11705-017-1664-9

摘要: Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

关键词: methanation     layered double hydroxide     bimetal Ni-Fe alloy     sintering     carbon deposition    

Crosslinking acrylamide with EDTA-intercalated layered double hydroxide for enhanced recovery of Cr(VI

Jing Li, Haiqin Yu, Xue Zhang, Rixin Zhu, Liangguo Yan

《环境科学与工程前沿(英文)》 2020年 第14卷 第3期 doi: 10.1007/s11783-020-1229-x

摘要: Functional groups of AM and EDTA in composite increased removal of Cr(VI) and CR. Removal process reached equilibrium within 30 min and was minimally affected by pH. Elimination of Cr(VI) was promoted by coexisting CR. Adsorption process of CR was less influenced by the presence of Cr(VI). Mechanisms were electrostatic attraction, surface complexation and anion exchange. We prepared ethylenediaminetetraacetic acid (EDTA)-intercalated MgAl-layered double hydroxide (LDH-EDTA), then grafted acrylamide (AM) to the LDH-EDTA by a cross-linking method to yield a LDH-EDTA-AM composite; we then evaluated its adsorptive ability for Congo red (CR) and hexavalent chromium (Cr(VI)) in single and binary adsorption systems. The adsorption process on LDH-EDTA-AM for CR and Cr(VI) achieved equilibrium quickly, and the removal efficiencies were minimally affected by initial pH. The maximum uptake quantities of CR and Cr(VI) on LDH-EDTA-AM were 632.9 and 48.47 mg/g, respectively. In mixed systems, chromate removal was stimulated by the presence of CR, while the adsorption efficiency of CR was almost not influenced by coexisting Cr(VI). The mechanisms involved electrostatic attraction, surface complexation, and anion exchange for the adsorption of both hazardous pollutants. In the Cr(VI) adsorption process, reduction also took place. The removal efficiencies in real contaminated water were all higher than those in the laboratory solutions.

关键词: Chromate     Dye adsorption     Simultaneous removal     Cross-linking method     Amino functionalization    

Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable

《化学科学与工程前沿(英文)》 2023年 第17卷 第1期   页码 102-115 doi: 10.1007/s11705-022-2179-6

摘要: High-performance and stable electrocatalysts are vital for the oxygen evolution reaction (OER). Herein, via a one-pot hydrothermal method, Ni/Fe/V ternary layered double hydroxides (NiFeV-LDH) derived from Ni foam are fabricated to work as highly active and durable electrocatalysts for OER. By changing the feeding ratio of Fe and V salts, the prepared ternary hydroxides were optimized. At an Fe:V ratio of 0.5:0.5, NiFeV-LDH exhibits outstanding OER activity superior to that of the binary hydroxides, requiring overpotentials of 269 and 274 mV at 50 mA·cm–2 in the linear sweep voltammetry and sampled current voltammetry measurements, respectively. Importantly, NiFeV-LDH shows extraordinary long-term stability (≥ 75 h) at an extremely high current density of 200 mA·cm–2. In contrast, the binary hydroxides present quick decay at 200 mA·cm–2 or even reduced current densities (150 and 100 mA·cm–2). The outstanding OER performance of NiFeV-LDH benefits from the synergistic effect of V and Fe while doping the third metal into bimetallic hydroxide layers: (a) Fe plays a crucial role as the active site; (b) electron-withdrawing V stabilizes the high valence state of Fe, thus accelerating the OER process; (c) V further offers great stabilization for the formed intermediate of FeOOH, thus achieving superior durability.

关键词: oxygen evolution reaction     electrocatalysts     ternary layered double hydroxides     long-term stability    

Hydraulic fracturing pressure of concentric double-layered cylinder in cohesive soil

《结构与土木工程前沿(英文)》 2021年 第15卷 第4期   页码 937-947 doi: 10.1007/s11709-021-0754-4

摘要: This study aims to investigate hydrofracturing in double-layered soil through theoretical and experimental analysis, as multilayered soils where the difference in mechanical properties exists are generally encountered in practical engineering. First, an analytical solution for fracturing pressure in two different concentric regions of soil was presented based on the cavity expansion theory. Then, several triaxial hydraulic fracturing tests were carried out to validate the analytical solution. The comparison between the experimental and analytical results indicates the remarkable accuracy of the derived formula, and the following conclusions were also obtained. First, there is a linear relationship between the fracturing pressure and confining pressure in concentric double-layered cohesive soil. Second, when the internal-layer soil is softer than the external-layer soil, the presence of internal soil on the fracturing pressure approximately brings the weakening effect, and the greater strength distinction between the two layers, the greater the weakening effect. Third, when the internal-layer soil is harder than the external-layer soil, the existence of the internal-layer soil has a strengthening effect on the fracturing pressure regardless of the proportion of internal-layer soil. Moreover, the influence of strength distinction between the two layers on the fracturing pressure is significant when the proportion of internal-layer soil is less than half, while it’s limited when the proportion is more than half. The proposed solution is potentially useful for geotechnical problems involving aspects of cohesive soil layering in a composite formation.

关键词: hydraulic fracturing pressure     layered     cavity expansion theory     triaxial fracturing test     cohesive soil    

Photocatalytic syngas synthesis from CO

Ling Tan, Kipkorir Peter, Jing Ren, Baoyang Du, Xiaojie Hao, Yufei Zhao, Yu-Fei Song

《化学科学与工程前沿(英文)》 2021年 第15卷 第1期   页码 99-108 doi: 10.1007/s11705-020-1947-4

摘要: The rational design of photocatalyst that can effectively reduce CO under visible light ( >400 nm), and simultaneously precise control of the products syngas (CO/H ) ratio is highly desirable for the Fischer-Tropsch reaction. In this work, we synthesized a series of CeO -decorated layered double hydroxides (LDHs, Ce- ) samples for photocatalytic CO reduction. It was found that the selectivity and productivity of CO and H from photoreduction of CO in conjunction with Ru-complex as photosensitizer performed an obvious “volcano-like” trend, with the highest point at Ce-0.15 and the CO/H ratio can be widely tunable from 1/7.7 to 1/1.3. Furthermore, compared with LDH, Ce-0.15 also drove photocatalytic CO to syngas under 600 nm irradiation. It implied that an optimum amount of CeO modifying LDH promoted the photoreduction of CO to syngas. This report gives the way to fully utilize the rare earth elements and provides a promising route to enhance the photo-response ability and charge injection efficiency of LDH-based photocatalysts in the synthesis of syngas with a tunable ratio under visible light irradiation.

关键词: visible light catalysis     CO2 conversion     layered double hydroxide     rare earth elements    

Crack evolution of soft–hard composite layered rock-like specimens with two fissures under uniaxial compression

《结构与土木工程前沿(英文)》 2021年 第15卷 第6期   页码 1372-1389 doi: 10.1007/s11709-021-0772-2

摘要: Acoustic emission and digital image correlation were used to study the spatiotemporal evolution characteristics of crack extension of soft and hard composite laminated rock masses (SHCLRM) containing double fissures under uniaxial compression. The effects of different rock combination methods and prefabricated fissures with different orientations on mechanical properties and crack coalescence patterns were analyzed. The characteristics of the acoustic emission source location distribution, and frequency changes of the crack evolution process were also investigated. The test results show that the damage mode of SHCLRM is related to the combination mode of rock layers and the orientation of fractures. Hard layers predominantly produce tensile cracks; soft layers produce shear cracks. The first crack always sprouts at the tip or middle of prefabricated fractures in hard layers. The acoustic emission signal of SHCLRM with double fractures has clear stage characteristics, and the state of crack development can be inferred from this signal to provide early warning for rock fracture instability. This study can provide a reference for the assessment of the fracture development status between adjacent roadways in SHCLRM in underground mines, as well as in roadway layout and support.

关键词: soft−hard composite layered rock mass     double cracks     crack evolution     acoustic emission     digital image correlation    

Stability analysis of layered slopes in unsaturated soils

Guangyu DAI; Fei ZHANG; Yuke WANG

《结构与土木工程前沿(英文)》 2022年 第16卷 第3期   页码 378-387 doi: 10.1007/s11709-022-0808-2

摘要: This study presents stability analyses of layered soil slopes in unsaturated conditions and uses a limit equilibrium method to determine the factor of safety involving suction stress of unsaturated soil. One-dimensional steady infiltration and evaporation conditions are considered in the stability analyses. An example of a two-layered slope in clay and silt is selected to verify the used method by comparing with the results of other methods. Parametric analyses are conducted to explore the influences of the matric suction on the stability of layered soil slopes. The obtained results show that larger suction stress provided in unsaturated clay dominates the stability of the layered slopes. Therefore, the location and thickness of the clay layer have significant influences on slope stability. As the water level decreases, the factor of safety reduces and then increases gradually in most cases. Infiltration/evaporation can obviously affect the stability of unsaturated layered slopes, but their influences depend on the soil property and thickness of the lower soil layer.

关键词: slope stability     suction stress     unsaturated soil     layered slope     limit equilibrium    

Synthesis and characterization of magnesium hydroxide by batch reaction crystallization

Xingfu SONG, Shuying SUN, Dengke ZHANG, Jin WANG, Jianguo YU

《化学科学与工程前沿(英文)》 2011年 第5卷 第4期   页码 416-421 doi: 10.1007/s11705-011-1125-9

摘要: Magnesium hydroxide with high purity and uniform particle size distribution was synthesized by the direct precipitation method using MgCl and NaOH as reactive materials and NaCl as additive to improve the crystallization behavior of the product. The particle size distribution, crystal phase, morphology, and surface area of magnesium hydroxide were characterized by Malvern laser particle size analyzer, X-ray diffraction (XRD), scanning electron microscope (SEM) and Branauer-Emmett-Teller (BET) method, respectively. The purity of products was analyzed by the chemical method. The effects of synthesis conditions on the particle size distribution and water content (filtration cake) of magnesium hydroxide were investigated. The results indicated that feeding mode and rate, and reaction temperature had important effects on water content and the particle size distribution of the product, and sodium chloride improved the crystallization behavior of magnesium hydroxide. The ball-like magnesium hydroxides with the particle size distribution of 6.0–30.0 μm and purity higher than 99.0% were obtained. This simple and mild synthesis method was promising to be scaled up for the industrial production of magnesium hydroxide.

关键词: magnesium hydroxide     direct precipitation method     industrial crystallization     particle size distribution    

Quantification of seepage in a multi-layered disconnected river-aquifer system

Jiang LI, Haizhu HU, Xiaomin MAO, Yi LIU

《农业科学与工程前沿(英文)》 2017年 第4卷 第2期   页码 237-245 doi: 10.15302/J-FASE-2017135

摘要: Quantification of seepage in disconnected river-aquifer systems is significant for local water management and groundwater pollution control, especially in areas with water shortage or contamination. The vadose zone under riverbeds usually exhibits a multi-layered structure, particularly when paved with low permeability liners. To evaluate the impact of engineering solutions to seepage under such conditions, we proposed an approach by combining GIS and the minimum flux in saturation layer (MFSL) method. MFSL can calculate the stable seepage rate by assessing the dominant low permeability layers (including but not limited to the liners) in multi-layered disconnected river-aquifer systems. We used MFSL to calculate local seepage rate, and used GIS to extend the results to a regional scale. The reliability of MFSL is discussed by comparing the results with the double ring infiltration test, the numerical simulation by HYDRUS, and the methods of stream package in MODFLOW, including its improved form. A case study was conducted in the Yongding River with river-aquifer seepage calculated under various conditions, including different river water levels (i.e., under the designated water level, drought stage level, flood stage level and flood inundation level) and with/without low permeability liners (i.e., ecological membranes or geomembrane). Results showed that low permeability liners could greatly reduce the seepage rate. However, if an unlined inundation area exists, the seepage rate may increase greatly. The results indicated that the proposed method was reliable and convenient for calculating long-term, large area seepage in disconnected river-aquifer systems especially those paved with liners.

关键词: infiltration     low permeability liner     multi-layered porous media     river-aquifer seepage    

Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

《化学科学与工程前沿(英文)》 2020年 第14卷 第6期   页码 948-955 doi: 10.1007/s11705-020-1920-2

摘要: Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions, including the oxygen evolution reaction (OER) and glucose oxidation reaction (GOR). Herein, we prepared cobalt hydroxide nanoparticles (CoHP) and cobalt hydroxide nanosheets (CoHS) on nickel foam. In the electrocatalytic OER, CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm . This is enhanced as compared with that of CoHP (367 mV at 10 mA·cm ). In addition, CoHS also exhibits an improved performance in the electrocatalytic GOR. The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer. These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.

关键词: electrocatalytic oxidation     cobalt hydroxide     nanosheet     water     glucose    

Size effects in two-dimensional layered materials modeled by couple stress elasticity

Wipavee WONGVIBOONSIN, Panos GOURGIOTIS, Chung Nguyen VAN, Suchart LIMKATANYU, Jaroon RUNGAMORNRAT

《结构与土木工程前沿(英文)》 2021年 第15卷 第2期   页码 425-443 doi: 10.1007/s11709-021-0707-y

摘要: In the present study, the effect of material microstructure on the mechanical response of a two-dimensional elastic layer perfectly bonded to a substrate is examined under surface loadings. In the current model, the substrate is treated as an elastic half plane as opposed to a rigid base, and this enables its applications in practical cases when the modulus of the layer (e.g., the coating material) and substrate (e.g., the coated surface) are comparable. The material microstructure is modeled using the generalized continuum theory of couple stress elasticity. The boundary value problems are formulated in terms of the displacement field and solved in an analytical manner via the Fourier transform and stiffness matrix method. The results demonstrate the capability of the present continuum theory to efficiently model the size-dependency of the response of the material when the external and internal length scales are comparable. Furthermore, the results indicated that the material mismatch and substrate stiffness play a crucial role in the predicted elastic field. Specifically, the study also addresses significant discrepancy of the response for the case of a layer resting on a rigid substrate.

关键词: cosserat     layered materials     size effects     microstructure    

New pseudo-dynamic analysis of two-layered cohesive-friction soil slope and its numerical validation

Suman HAZARI, Sima GHOSH, Richi Prasad SHARMA

《结构与土木工程前沿(英文)》 2020年 第14卷 第6期   页码 1492-1508 doi: 10.1007/s11709-020-0679-3

摘要: Natural slopes consist of non-homogeneous soil profiles with distinct characteristics from slopes made of homogeneous soil. In this study, the limit equilibrium modified pseudo-dynamic method is used to analyze the stability of two-layered soil slopes in which the failure surface is assumed to be a logarithmic spiral. The zero-stress boundary condition at the ground surface under the seismic loading condition is satisfied. New formulations derived from an analytical method are proposed for the predicting the seismic response in two-layered soil. A detailed parametric study was performed in which various parameters (seismic accelerations, damping, cohesion, and angle of internal friction) were varied. The results of the present method were compared with those in the available literature. The present analytical analysis was also verified against the finite element analysis results.

关键词: layered soil     limit equilibrium method     seismic analysis     damping     PLAXIS    

标题 作者 时间 类型 操作

Hierarchically porous cellulose nanofibril aerogel decorated with polypyrrole and nickel-cobalt layereddouble hydroxide for high-performance nonenzymatic glucose sensors

期刊论文

Defective Nickle–Iron Layered Double Hydroxide for Enhanced Photocatalytic NO Oxidation with Significant

Xiaoyu Li,Xiaoshu Lv,Jian Pan,Peng Chen,Huihui Peng,Yan Jiang,Haifeng Gong,Guangming Jiang,Li'an Hou,

期刊论文

Layered double hydroxide-based core-shell nanoarrays for efficient electrochemical water splitting

Wenfu Xie, Zhenhua Li, Mingfei Shao, Min Wei

期刊论文

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

期刊论文

Crosslinking acrylamide with EDTA-intercalated layered double hydroxide for enhanced recovery of Cr(VI

Jing Li, Haiqin Yu, Xue Zhang, Rixin Zhu, Liangguo Yan

期刊论文

Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable

期刊论文

Hydraulic fracturing pressure of concentric double-layered cylinder in cohesive soil

期刊论文

Photocatalytic syngas synthesis from CO

Ling Tan, Kipkorir Peter, Jing Ren, Baoyang Du, Xiaojie Hao, Yufei Zhao, Yu-Fei Song

期刊论文

Crack evolution of soft–hard composite layered rock-like specimens with two fissures under uniaxial compression

期刊论文

Stability analysis of layered slopes in unsaturated soils

Guangyu DAI; Fei ZHANG; Yuke WANG

期刊论文

Synthesis and characterization of magnesium hydroxide by batch reaction crystallization

Xingfu SONG, Shuying SUN, Dengke ZHANG, Jin WANG, Jianguo YU

期刊论文

Quantification of seepage in a multi-layered disconnected river-aquifer system

Jiang LI, Haizhu HU, Xiaomin MAO, Yi LIU

期刊论文

Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

期刊论文

Size effects in two-dimensional layered materials modeled by couple stress elasticity

Wipavee WONGVIBOONSIN, Panos GOURGIOTIS, Chung Nguyen VAN, Suchart LIMKATANYU, Jaroon RUNGAMORNRAT

期刊论文

New pseudo-dynamic analysis of two-layered cohesive-friction soil slope and its numerical validation

Suman HAZARI, Sima GHOSH, Richi Prasad SHARMA

期刊论文