A critical review on thermodynamic mechanisms of membrane fouling in membrane-based water treatment process

● Fundamentals of membrane fouling are comprehensively reviewed. ● Contribution of thermodynamics on revealing membrane fouling mechanism is summarized. ● Quantitative approaches toward thermodynamic fouling mechanisms are deeply analyzed. ● Inspirations of thermodynamics for membrane fouling mitigation are briefly discussed. ● Research prospects on thermodynamics and membrane fouling are forecasted. Membrane technology is widely regarded as one of the most promising technologies for wastewater treatment and reclamation in the 21st century. However, membrane fouling significantly limits its applicability and productivity. In recent decades, research on the membrane fouling has been one of the hottest spots in the field of membrane technology. In particular, recent advances in thermodynamics have substantially widened people’s perspectives on the intrinsic mechanisms of membrane fouling. Formulation of fouling mitigation strategies and fabrication of anti-fouling membranes have both benefited substantially from those studies. In the present review, a summary of the recent results on the thermodynamic mechanisms associated with the critical adhesion and filtration processes during membrane fouling is provided. Firstly, the importance of thermodynamics in membrane fouling is comprehensively assessed. Secondly, the quantitative methods and general factors involved in thermodynamic fouling mechanisms are critically reviewed. Based on the aforementioned information, a brief discussion is presented on the potential applications of thermodynamic fouling mechanisms for membrane fouling control. Finally, prospects for further research on thermodynamic mechanisms underlying membrane fouling are presented. Overall, the present review offers comprehensive and in-depth information on the thermodynamic mechanisms associated with complex fouling behaviors, which will further facilitate research and development in membrane technology.     

Enhanced cross-flow filtration with flat-sheet ceramic membranes by titanium-based coagulation for membrane fouling control

• Ceramic membrane filtration showed high performance for surface water treatment. • PTC pre-coagulation could enhance ceramic membrane filtration performance. • Ceramic membrane fouling was investigated by four varied mathematical models. • PTC pre-coagulation was high-effective for ceramic membrane fouling control. Application of ceramic membrane (CM) with outstanding characteristics, such as high flux and chemical-resistance, is inevitably restricted by membrane fouling. Coagulation was an economical and effective technology for membrane fouling control. This study investigated the filtration performance of ceramic membrane enhanced by the emerging titanium-based coagulant (polytitanium chloride, PTC). Particular attention was paid to the simulation of ceramic membrane fouling using four widely used mathematical models. Results show that filtration of the PTC-coagulated effluent using flat-sheet ceramic membrane achieved the removal of organic matter up to 78.0%. Permeate flux of ceramic membrane filtration reached 600 L/(m²·h), which was 10-fold higher than that observed with conventional polyaluminum chloride (PAC) case. For PTC, fouling of the ceramic membrane was attributed to the formation of cake layer, whereas for PAC, standard filtration/intermediate filtration (blocking of membrane pores) was also a key fouling mechanism. To sum up, cross-flow filtration with flat-sheet ceramic membranes could be significantly enhanced by titanium-based coagulation to produce both high-quality filtrate and high-permeation flux.     

Metabolic uncoupler, 3,3′,4′,5-tetrachlorosalicylanilide addition for sludge reduction and fouling control in a gravity-driven membrane bioreactor

• Effects of metabolic uncoupler TCS on the performances of GDMBR were evaluated. • Sludge EPS reduced and transformed into dissolved SMP when TCS was added. • Appropriate TCS increased the permeability and reduced cake layer fouling. • High dosage aggravated fouling due to compact cake layer with low bio-activity. The gravity-driven membrane bioreactor (MBR)system is promising for decentralized sewage treatment because of its low energy consumption and maintenance requirements. However, the growing sludge not only increases membrane fouling, but also augments operational complexities (sludge discharge). We added the metabolic uncoupler 3,3′,4′,5-tetrachlorosalicylanilide (TCS) to the system to deal with the mentioned issues. Based on the results, TCS addition effectively decreased sludge ATP and sludge yield (reduced by 50%). Extracellular polymeric substances (EPS; proteins and polysaccharides) decreased with the addition of TCS and were transformed into dissolved soluble microbial products (SMPs) in the bulk solution, leading to the break of sludge flocs into small fragments. Permeability was increased by more than two times, reaching 60–70 L/m²/h bar when 10–30 mg/L TCS were added, because of the reduced suspended sludge and the formation of a thin cake layer with low EPS levels. Resistance analyses confirmed that appropriate dosages of TCS primarily decreased the cake layer and hydraulically reversible resistances. Permeability decreased at high dosage (50 mg/L) due to the release of excess sludge fragments and SMP into the supernatant, with a thin but more compact fouling layer with low bioactivity developing on the membrane surface, causing higher cake layer and pore blocking resistances. Our study provides a fundamental understanding of how a metabolic uncoupler affects the sludge and bio-fouling layers at different dosages, with practical relevance for in situ sludge reduction and membrane fouling alleviation in MBR systems.     

苦咸水反渗透淡化中影响膜面的污染因素

由于苦咸水的化学组成和浓度分布在不同地区有着显著的差异,以及淡化工艺中普遍较高的浓缩因子(concentrate factor,CF)值(在4—10之间),苦咸水反渗透(brackish water reverse osmosis,BWRO)淡化过程中的膜污染现象、类型和程度较海水反渗透(seawater reverse osmosis,SWRO)淡化过程有明显的不同.目前,膜污染已成为BWRO大规模应用于苦咸水淡化领域的瓶颈之一,如何解决这一问题成为该领域的研究热点.本文详细综述了国内外BWRO淡化过程中影响膜面污染因素的应用研究进展,重点介绍了进水来源污染成分及污染倾向、进水水质优劣指标和进水物性对膜面污染的影响;按照分离技术的不同,分类讨论了常规预处理和膜法预处理工艺,指出后者不易受进水水质变化的影响,能够更好地降低膜面污染潜能,并针对目前的研究现状提出了建议.     

Ceramic water filter for point-of-use water treatment in developing countries: Principles,challenges and opportunities

• CWF is a sustainable POU water treatment method for developing areas. • CWF manufacturing process is critical for its filtration performance. • Simultaneous increase of flow rate and pathogen removal is a challenge. • Control of pore size distribution holds promises to improve CWF efficiency. • Novel coatings of CWFs are a promising method to improve contaminant removal. Drinking water source contamination poses a great threat to human health in developing countries. Point-of-use (POU) water treatment techniques, which improve drinking water quality at the household level, offer an affordable and convenient way to obtain safe drinking water and thus can reduce the outbreaks of waterborne diseases. Ceramic water filters (CWFs), fabricated from locally sourced materials and manufactured by local labor, are one of the most socially acceptable POU water treatment technologies because of their effectiveness, low-cost and ease of use. This review concisely summarizes the critical factors that influence the performance of CWFs, including (1) CWF manufacturing process (raw material selection, firing process, silver impregnation), and (2) source water quality. Then, an in-depth discussion is presented with emphasis on key research efforts to address two major challenges of conventional CWFs, including (1) simultaneous increase of filter flow rate and bacterial removal efficiency, and (2) removal of various concerning pollutants, such as viruses and metal(loid)s. To promote the application of CWFs, future research directions can focus on: (1) investigation of pore size distribution and pore structure to achieve higher flow rates and effective pathogen removal by elucidating pathogen transport in porous ceramic and adjusting manufacture parameters; and (2) exploration of new surface modification approaches with enhanced interaction between a variety of contaminants and ceramic surfaces.     

Co-application of energy uncoupling and ultrafiltration in sludge treatment: Evaluations of sludge reduction,supernatant recovery and membrane fouling control

• Effects of metabolic uncouplers addition on sludge reduction were carried out. • TCS addition effectively inhibited ATP synthesis and reduced sludge yield. • The effluent quality such as TOC and ammonia deteriorated but not significantly. • Suitable dosage retarded biofouling during sludge water recovery by UF membrane. Energy uncoupling is often used for sludge reduction because it is easy to operate and does not require a significant amount of extra equipments (i.e. no additional tank required). However, over time the supernatant extracted using this method can deteriorate, ultimately requiring further treatment. The purpose of this study was to determine the effect of using a low-pressure ultrafiltration membrane process for sludge water recovery after the sludge had undergone an energy uncoupling treatment (using 3,3′,4′,5-tetrachlorosalicylanilide (TCS)). Energy uncoupling was found to break apart sludge floc by reducing extracellular polymeric substances (EPS) and adenosine triphosphate (ATP) content. Analysis of supernatant indicated that when energy uncoupling and membrane filtration were co-applied and the TCS dosage was below 30 mg/L, there was no significant deterioration in organic component removal. However, ammonia and phosphate concentrations were found to increase as the concentration of TCS added increased. Additionally, due to low sludge concentrations and EPS contents, addition of 30–60 mg/L TCS during sludge reduction increased the permeate flux (two times higher than the control) and decreased the hydraulic reversible and cake layer resistances. In contrast, high dosage of TCS aggravated membrane fouling by forming compact fouling layers. In general, this study found that the co-application of energy uncoupling and membrane filtration processes represents an effective alternative method for simultaneous sludge reduction and sludge supernatant recovery.     

Effect of chemical dose on phosphorus removal and membrane fouling control in a UCT-MBR

Phosphorus removal was enhanced effectively by dosing aluminum sulfate and effluent phosphorus concentration was lower than 0.5 mg/L. Sludge activity was not inhibited but improved slightly with addition of aluminum sulfate. EPS concentrations both in mixed liquid and on membrane surface were decreased, contributing to the effective mitigation of membrane fouling. To enhance phosphorus removal and make the effluent meet the strict discharge level of total phosphorus (TP, 0.5 mg/L), flocculant dosing is frequently applied. In this study, the performance of aluminum sulfate dosing in a University of Cape Town Membrane Bioreactor (UCT-MBR) was investigated, in terms of the nutrients removal performance, sludge characteristics and membrane fouling. The results indicated that the addition of aluminum sulfate into the aerobic reactor continuously had significantly enhanced phosphorus removal. Moreover, COD, NH₄⁺-N and TN removal were not affected and effluent all met the first level A criteria of GB18918-2002. In addition, the addition of aluminum sulfate had improved the sludge activity slightly and reduced trans-membrane pressure (TMP) increase rate from 1.13 KPa/d to 0.57 KPa/d effectively. The membrane fouling was alleviated attributed to the increased average particle sizes and the decreased accumulation of the small sludge particles on membrane surface. Furthermore, the decline of extracellular polymeric substance (EPS) concentration in mixed sludge liquid decreased its accumulation on membrane surface, resulting in the mitigation of membrane fouling directly.     

Aggravation of membrane fouling and methane leakage by a three-phase separator in an external anaerobic ceramic membrane bioreactor

The existence of three-phase separator did not affect COD removal in the EAnCMBR. The existence of three-phase separator aggravated methane leakage of EAnCMBR. The existence of three-phase separator aggravated membrane fouling rate of EAnCMBR. Start-up of EAnCMBR equipped three-phase separator was slightly delayed. The three-phase separator is a critical component of high-rate anaerobic bioreactors due to its significant contribution in separation of biomass, wastewater, and biogas. However, its role in an anaerobic membrane bioreactor is still not clear. In this study, the distinction between an external anaerobic ceramic membrane bioreactor (EAnCMBR) unequipped (R1) and equipped (R2) with a three-phase separator was investigated in terms of treatment performance, membrane fouling, extracellular polymers of sludge, and microbial community structure. The results indicate that the COD removal efficiencies of R1 and R2 were 98.2%±0.4% and 98.1%±0.4%, respectively, but the start-up period of R2 was slightly delayed. Moreover, the membrane fouling rate of R2 (0.4 kPa/d) was higher than that of R1 (0.2 kPa/d). Interestingly, the methane leakage from R2 (0.1 L/d) was 20 times higher than that from R1 (0.005 L/d). The results demonstrate that the three-phase separator aggravated the membrane fouling rate and methane leakage in the EAnCMBR. Therefore, this study provides a novel perspective on the effects of a three-phase separator in an EAnCMBR.     

Experimental and computational assessment of 1,4-Dioxane degradation in a photo-Fenton reactive ceramic membrane filtration process

• 1,4-Dioxane was degraded via the photo-Fenton reactive membrane filtration. • Degradation efficiency and AQY were both enhanced in photocatalytic membrane. • There is a tradeoff between photocatalytic degradation and membrane permeation flux. • Degradation pathways of 1,4-Dioxane is revealed by DFT analysis. The present study evaluated a photo-Fenton reactive membrane that achieved enhanced 1,4-Dioxane removal performance. As a common organic solvent and stabilizer, 1,4-Dioxane is widely used in a variety of industrial products and poses negative environmental and health impacts. The membrane was prepared by covalently coating photocatalyst of goethite (α-FeOOH) on a ceramic porous membrane as we reported previously. The effects of UV irradiation, H₂O₂ and catalyst on the removal efficiency of 1,4-Dioxane in batch reactors were first evaluated for optimized reaction conditions, followed by a systematical investigation of 1,4-Dioxane removal in the photo-Fenton membrane filtration mode. Under optimized conditions, the 1,4-Dioxane removal rate reached up to 16% with combination of 2 mmol/L H₂O₂ and UV₃₆₅ irradiation (2000 µW/cm²) when the feed water was filtered by the photo-Fenton reactive membrane at a hydraulic retention time of 6 min. The removal efficiency and apparent quantum yield (AQY) were both enhanced in the filtration compared to the batch mode of the same photo-Fenton reaction. Moreover, the proposed degradation pathways were analyzed by density functional theory (DFT) calculations, which provided a new insight into the degradation mechanisms of 1,4-Dioxane in photo-Fenton reactions on the functionalized ceramic membrane.     

Design of nanofibre interlayer supported forward osmosis composite membranes and its evaluation in fouling study with cleaning

• A fine fibre (40–60 nm diameter) interlayer (~1 µm thickness) was electrospun. • Fine fibre interlayer promoted formation of defect-free dense polyamide layer. • FO membrane with dual-layer substrate had less organic fouling potential. • High reverse salt flux accelerated organic fouling on FO membrane. Nanofibre-supported forward osmosis (FO) membranes have gained popularity owing to their low structural parameters and high water flux. However, the nanofibrous membranes are less stable in long-term use, and their fouling behaviours with foulants in both feed solution (FS) and draw solution (DS) is less studied. This study developed a nanofibrous thin-film composite (TFC) FO membrane by designing a tiered dual-layer nanofibrous substrate to enhance membrane stability during long-term usage and cleaning. Various characterisation methods were used to study the effect of the electrospun nanofibre interlayer and drying time, which is the interval after removing the M-phenylenediamine (MPD) solution and before reacting with trimesoyl chloride (TMC) solution, on the intrinsic separation FO performance. The separation performance of the dual-layer nanofibrous FO membranes was examined using model foulants (sodium alginate and bovine serum albumin) in both the FS and DS. The dual-layer nanofibrous substrate was superior to the single-layer nanofibrous substrate and showed a flux of 30.2 L/m²/h (LMH) when using 1.5 mol/L NaCl against deionised (DI) water in the active layer facing draw solution (AL-DS) mode. In the fouling test, the water flux was effectively improved without sacrificing the water/solute selectivity under the condition that foulants existed in both the FS and DS. In addition, the dual-layer nanofibrous TFC FO membrane was more robust during the fouling test and cleaning.     

Simultaneously recovering electricity and water from wastewater by osmotic microbial fuel cells: Performance and membrane fouling

Since the concept of the osmotic microbial fuel cell (OsMFC) was introduced in 2011, it has attracted growing interests for its potential applications in wastewater treatment and energy recovery. However, forward osmosis (FO) membrane fouling resulting in a severe water flux decline remains a main obstacle. Until now, the fouling mechanisms of FO membrane especially the development of biofouling layer in the OsMFC are not yet clear. Here, the fouling behavior of FO membrane in OsMFCs was systematically investigated. The results indicated that a thick fouling layer including biofouling and inorganic fouling was existed on the FO membrane surface. Compared to the inorganic fouling, the biofouling played a more important role in the development of the fouling layer. Further analyses by the confocal laser scanning microscopy (CLSM) implied that the growth of biofouling layer on the FO membrane surface in the OsMFC could be divided into three stages. Initially, microorganisms associated with ß-D-glucopyranose polysaccharides were deposited on the FO membrane surface. After that, the microorganisms grew into a biofilm caused a quick decrease of water flux. Subsequently, some of microorganisms were dead due to lack of nutrient source, in the meantime, polysaccharide and proteins in the biofouling layer were decomposed as nutrient source, thus leading to a slow development of the biofouling layer. Moreover, the microorganisms played a significant role in the formation and development of the biofouling layer, and further studies are needed to mitigate the deposition of microorganisms on FO membrane surfaces in OsMFCs.

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Recent advances in membrane bioreactor technology for wastewater treatment in China

Since the introduction of the membrane bioreactor (MBR) in China in the early 1990s, remarkable progress has been achieved on the research and application of this technology. China has now become one of the most active fields in the world in this regard. This review outlines the development of MBR-based processes in China and their performance of treating municipal and industrial wastewaters. Since membrane fouling is a critical operational problem with MBR processes, this paper also proposes updated understanding of fouling mechanisms and strategies of fouling control, which are mainly compiled from publications of Chinese researchers. As for the commercial application of MBR in the country, the latest statistics of large-scale MBR plants (>10000 m³·d⁻¹) are provided, and the growth trend of total treatment capacity as well as its driving force is analyzed.     

Hydroxyl radical intensified Cu2O NPs/H2O2 process in ceramic membrane reactor for degradation on DMAc wastewater from polymeric membrane manufacturer

• Cu₂O NPs/H₂O₂ Fenton process was intensified by membrane dispersion. • DMAc removal was enhanced to 98% for initial DMAc of 14000 mg/L. • Analyzed time-resolved degradation pathway of DMAc under ·OH attack. High-concentration industrial wastewater containing N,N-dimethylacetamide (DMAc) from polymeric membrane manufacturer was degraded in Cu₂O NPs/H₂O₂ Fenton process. In the membrane-assisted Fenton process DMAc removal rate was up to 98% with 120 min which was increased by 23% over the batch reactor. It was found that ·OH quench time was extended by 20 min and the maximum ·OH productivity was notably 88.7% higher at 40 min. The degradation reaction rate constant was enhanced by 2.2 times with membrane dispersion (k = 0.0349 min⁻¹). DMAc initial concentration (C₀) and H₂O₂ flux (J_p) had major influence on mass transfer and kinetics, meanwhile, membrane pore size (r_p) and length (L_m) also affected the reaction rate. The intensified radical yield, fast mass transfer and nanoparticles high activity all contributed to improve pollutant degradation efficiency. Time-resolved DMAc degradation pathway was analyzed as hydroxylation, demethylation and oxidation leading to the final products of CO₂, H₂O and NO₃⁻ (rather than NH₃ from biodegradation). Continuous process was operated in the dual-membrane configuration with in situ reaction and separation. After five cycling tests, DMAc removal was all above 95% for the initial [DMAc]₀ = 14,000 mg/L in wastewater and stability of the catalyst and the membrane maintained well.     

Effect of protein on PVDF ultrafiltration membrane fouling behavior under different pH conditions: interface adhesion force and XDLVO theory analysis

To further determine the fouling behavior of bovine serum albumin (BSA) on different hydrophilic PVDF ultrafiltration (UF) membranes over a range of pH values, self-made atomic force microscopy (AFM) colloidal probes were used to detect the adhesion forces of membrane–BSA and BSA–BSA, respectively. Results showed that the membrane–BSA adhesion interaction was stronger than the BSA–BSA adhesion interaction, and the adhesion force between BSA–BSA-fouled PVDF/PVA membranes was similar to that between BSA–BSA-fouled PVDF/PVP membranes, which indicated that the fouling was mainly caused by the adhesion interaction between membrane and BSA. At the same pH condition, the PVDF/PVA membrane–BSA adhesion force was smaller than that of PVDF/ PVP membrane–BSA, which illustrated that the more hydrophilic the membrane was, the better antifouling ability it had. The extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory predicts that the polar or Lewis acid–base (AB) interaction played a dominant role in the interfacial free energy of membrane–BSA and BSA–BSA that can be affected by pH. For the same membrane, the pH values of a BSA solution can have a significant impact on the process of membrane fouling by changing the AB component of free energy.

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Comparison of CNT-PVA membrane and commercial polymeric membranes in treatment of emulsified oily wastewater

CNT-PVA membrane was fabricated and compared with polymeric membranes. The separation performance was evaluated by homemade and cutting fluid emulsions. The three membranes show similar oil retention rates. CNT-PVA membranes have higher permeation fluxes compared with polymeric membranes. CNT-PVA membrane shows higher fouling resistance. Membrane separation is an attractive technique for removal of emulsified oily wastewater. However, polymeric membranes which dominate the current market usually suffer from severe membrane fouling. Therefore, membranes with high fouling resistance are imperative to treat emulsified oily wastewater. In this study, carbon nanotube-polyvinyl alcohol (CNT-PVA) membrane was fabricated. And its separation performance for emulsified oily wastewater was compared with two commercial polymeric membranes (PVDF membrane and PES membrane) by filtration of two homemade emulsions and one cutting fluid emulsion. The results show that these membranes have similar oil retention efficiencies for the three emulsions. Whereas, the permeation flux of CNT-PVA membrane is 1.60 to 3.09 times of PVDF membrane and 1.41 to 11.4 times of PES membrane, respectively. Moreover, after five consecutive operation circles of filtration process and back flush, CNT-PVA membrane can recover 62.3% to 72.9% of its initial pure water flux. However, the pure water flux recovery rates are only 24.1% to 35.3% for PVDF membrane and 6.0% to 26.3% for PES membrane, respectively. Therefore, CNT-PVA membrane are more resistant to oil fouling compared with the two polymeric membranes, showing superior potential in treatment of emulsified oily wastewater.     

Using loose nanofiltration membrane for lake water treatment: A pilot study

• A pilot study was conducted for drinking water treatment using loose NF membranes. • The membranes had very high rejection of NOM and medium rejection of Ca²⁺/Mg²⁺. • Organic fouling was dominant and contribution of inorganic fouling was substantial. • Both organic and inorganic fouling had spatial non-uniformity on membrane surface. • Applying EDTA at basic conditions was effective in removing membrane fouling. Nanofiltration (NF) using loose membranes has a high application potential for advanced treatment of drinking water by selectively removing contaminants from the water, while membrane fouling remains one of the biggest problems of the process. This paper reported a seven-month pilot study of using a loose NF membrane to treat a sand filtration effluent which had a relatively high turbidity (~0.4 NTU) and high concentrations of organic matter (up to 5 mg/L as TOC), hardness and sulfate. Results showed that the membrane demonstrated a high rejection of TOC (by>90%) and a moderately high rejection of two pesticides (54%–82%) while a moderate rejection of both calcium and magnesium (~45%) and a low rejection of total dissolved solids (~27%). The membrane elements suffered from severe membrane fouling, with the membrane permeance decreased by 70% after 85 days operation. The membrane fouling was dominated by organic fouling, while biological fouling was moderate. Inorganic fouling was mainly caused by deposition of aluminum-bearing substances. Though inorganic foulants were minor contents on membrane, their contribution to overall membrane fouling was substantial. Membrane fouling was not uniform on membrane. While contents of organic and inorganic foulants were the highest at the inlet and outlet region, respectively, the severity of membrane fouling increased from the inlet to the outlet region of membrane element with a difference higher than 30%. While alkaline cleaning was not effective in removing the membrane foulants, the use of ethylenediamine tetraacetate (EDTA) at alkaline conditions could effectively restore the membrane permeance.     

Natural control mechanisms in models of aquatic ecosystems

Based on cybernetic categories of natural control mechanisms, four generations of ecosystem models are distinguished: feed-forward, feedback, self-adaptation and self-organization models. The analysis of the natural control mechanisms in aquatic ecosystems suggests that different processes are controlled in different ways, and, although the four mechanisms were identified in historical sequence, they all operate simultaneously. The concept of self-organization of an ecosystem is introduced and specified for a model of an aquatic pelagic ecosystem. The concept of the ecosystem as a multilayer, multigoal and multiechelon hierarchical system with hierarchy of the levels of biological organization is also introduced.     

套种模式对水土保持效应的影响

在东江中上游低效水土保持林的改造中,营建了不同套种模式的水保林,效益监测结果表明,乔灌草模式、乔灌模式和马尾松纯林模式中,以乔灌草模式的水土保持效果为最佳.乔、灌、草层分别对降水的截留和吸附,以及大量的地上枯落物具有强大的持水能力,有效地减少了雨滴直接冲刷地表,使得乔灌草模式的土壤侵蚀明显减少,套种4 a后土壤侵蚀模数降为960 t/(km2(a),约为乔灌模式的1/3和马尾松纯林的1/5;同时使土壤蓄水能力提高,土壤肥力状况得到改善.