The removal of heavy metal ions and medical antibiotics from wastewater is crucial for environmental protection and human health. However, the adsorption capacities and reusability of previously reported adsorbent materials have been insufficient for efficient and sustainable wastewater treatment. In this study, we present a composite material, UiO-66-AMP@PAN, synthesized from metal-organic frameworks (MOFs) and polyacrylonitrile (PAN), which exhibits superior adsorption properties and reusability. The material demonstrates excellent adsorption capacities for heavy metal ions Pb(II) and Cr(VI) as well as the antibiotic tetracycline hydrochloride (TCH), among which the maximum adsorption capacities for Pb(II)(pH=7) and Cr(VI)(pH=5) and antibiotic tetracycline hydrochloride (TCH) (pH=9) were 455.8 mg/g, 442.08 mg/g and 405.92 mg/g, respectively. The adsorption efficiency of UiO-66-AMP@PAN as an adsorbent for adsorbing Pb(II)(pH=7) and Cr(VI)(pH=5) and the antibiotic tetracycline hydrochloride (TCH) (pH=9) remained above 90% even after ten consecutive cycles. The performance of UiO-66-AMP@PAN as an adsorbent has remained unchanged across multiple adsorption-desorption cycles, demonstrating its potential for long-term use in wastewater treatment applications. This innovative approach paves the way for the development of more efficient and environmentally friendly adsorption materials to address the challenges posed by heavy metal ions in wastewater and medical antibiotics.

The current study aims to develop a cost-effective and efficient treatment method for the remediation of amine-containing real industrial effluent. The method consists of a precipitation to remove chloride ions and TDS, followed by cavitation-based AOPs involving US and chemical oxidants as H2O2, O3, Fenton’s reagent, NaClO, and nTiO2. Different parameters including precipitating agent type and dosage, oxidant loading/flow rate, and time were assessed to determine optimal conditions for effective treatment. Treatment schemes were evaluated based on cavitational yield (mg/J), treatment cost (Rs/L), and COD reduction to select an industrially feasible design for amine-containing real effluent treatment. The optimum conditions elucidated were H2O2 loading of 3 g/L, NaClO loading of 3 g/L, O3 flowrate of 3 LPH, nTiO2 loading of 3 g/L, Fenton’s reagent ratio (H2O2/Fe2+) as 6:1. Under the optimum conditions, US+nTiO2 (70%) treatment schemes were the most efficient, achieving a maximum COD reduction compared to US+Fenton (65%), US+H2O2 (36%), US+O3 (49%) and US+NaClO (53%) schemes. Additionally, impact of chloride and TDS on the oxidation process in terms of COD reduction was assessed. Using Rotavap instead of precipitation, and subsequent use of the best oxidation method (US/HC+Fenton+CaO) achieved COD and TDS levels below 250 mg/L (discharge limit) at optimum conditions, with minimal operating costs of 0.23 $/L and 0.15 $/L, respectively. Overall, the study concluded that the sequential approach of precipitation/Rotavap and cavitation-assisted oxidation is an effective and sustainable method, providing a promising solution for the wastewater treatment in the metallurgical industry.

Electrochemical membrane filtration (EMF) is a promising advanced oxidation technology for eliminating aquatic refractory pharmaceuticals. In this work, three porous foam-titanium based metal oxide (MOx) anodic membranes were prepared for comparison of their effectiveness against the model pharmaceutical pollutant metoprolol. The electrooxidation efficiencies of metoprolol by all flow-by operated anodic membranes were found to be elevated with increasing charging voltage and decreasing electrolyte solution pH, in which the PbO2 membrane exhibited more efficient metoprolol degradation efficiency over SnO2 and RuO2 membranes. At the chosen charging voltage of 2 V and electrolyte solution pH 7, compared to the flow-by mode, the higher total organic carbon (TOC) removal and less electrical energy consumption was achieved by the flow-through operated PbO2 membrane, ascribed to the enhanced mass-transfer of metoprolol and its intermediate by-products toward the anode surface. The physisorbed and free HO• produced by PbO2 membrane were found to be the key oxidants accounting for metoprolol degradation, which induced the transformation of metoprolol by attacking its benzene ring and side chains. Apart from the capacity for detoxifying metoprolol-containing influent, PbO2 membrane also exhibited favorable stability in flow-through mode. The study provides an effective strategy for the electrochemical remediation of pharmaceutical-polluted water and wastewater.Data availabilityData will be made available on request.

The severe adverse impacts of the frequently occurring marine oil spills call for the urgent development of an efficient approach for oil spill restoration. Here, we prepared a superhydrophobic melamine sponge with water contact angle of 151.6° via a one-step dip-coating process by simply reacting the melamine sponge with stearic anhydride. The as-prepared sponge, MS-4, demonstrates excellent sorption capacities for various organic solvents such as hexane, toluene and chloroform, as well as oils including diesel, mineral oil, and crude oil, with sorption capacities ranging from 78 to 160 times its own mass. Moreover, MS-4 exhibits good recyclability with retention rate of over 93% even after 50 sorption/squeezing cycles, remarkable stability when exposed to challenging conditions such as strong acidic (pH = 1.0) and alkaline (pH = 13.0) environments, as well as high salinity environments. Additionally, MS-4 displays superb selectivity, enabling the continuous oil/water separation when assisted by a vacuum pump, achieving a high flux of approximately 106 L•m-2•h-1, while maintaining a low water content of as minimal as 30 ppm. Notably, through a facile filtration process, MS-4 achieves an exceptional demulsification efficiency of up to 99.7% for water-in-oil emulsions.

Controlling the formation of disinfection byproducts (DBPs) requires prior knowledge of DBP formation potential. Mathematical models can accurately predict the formation of DBPs and have the advantage of reducing laboratory tests and related costs. Researchers continue to develop new models for specific regions but rarely used external data sets to evaluate the predictive ability of previous models. Most of the models focus on total trihalomethanes (THMs), and the predictive models for emerging DBPs (e.g., chloral hydrate (CH)) are lacking. Moreover, little discussion is available on comparing linear and machine learning (ML) algorithms in predicting the formation of DBPs. This study investigated the predictive models of CH, chloroform, THMs, dichloroacetic acid, trichloroacetic acid, and haloacetic acids based on stepwise multiple linear regression and ML regression using easily monitored water quality parameters (i.e., pH, UV254, and total organic carbon (TOC)). Among these parameters, UV254 is the dominant parameter in predicting the formation of target DBPs and deserves more attention in future studies. Among the models for the target DBPs, the model for CH using stepwise multiple linear regression was shown as follows: LnCH = 8.945 + 0.558 × Ln(UV254) – 2.37 × Ln(pH) + 0.152 × Ln(TOC). The support vector regression (MAPE = 2.578–5.798%, R2 = 0.665–0.802) and random forest regression (MAPE = 2.867–5.346%, R2 = 0.671–0.965) performed better than traditional stepwise linear regression (MAPE = 2.857–6.671%, R2 = 0.602–0.770) in the training and testing set. This emphasized that ML algorithms were viable alternatives to conventional linear regression in the management of DBPs.

In recent years, chloroquine phosphate (CQP) has been widely used as a specific drug for treating COVID-19. Because of its biological toxicity, the release of CQP into water is bound to have a potential impact on human health. It is urgent to find a reusable and efficient catalyst to treat a large number of CQP wastewater. Currently, perovskite-type catalysts are gradually entering the field of advanced oxidation process, but there are still some problems such as high particle aggregation and limited reaction contact. Here, LaCo0.5Cu0.5O3-CeO2 was prepared by sol-gel method and used to activate peroxymonosulfate (PMS) to degrade CQP for the first time. The LaCo0.5Cu0.5O3-CeO2 material has better stability, larger specific surface area and more uniform pore structure. Under the conditions of 0.2 g/L catalyst and 1.0 mM PMS, 20 mg/L CQP can be completely degraded within 8 min and is suitable for a wide pH range and complex water quality. Superoxide free radical (·O2-) and the singlet oxygen (1O2) are the main free radicals to degrade CQP. The addition of CeO2 makes Ce4+/Ce3+ participate in the redox cycles between Co3+/Co2+ and Cu2+/Cu+, realizing the multipath electron transfer. In addition, LaCo0.5Cu0.5O3-CeO2/PMS system can degrade CQP into low toxicity products through different pathways, ultimately mineralizing it into inorganic small molecules. In general, LaCo0.5Cu0.5O3-CeO2 has more reasonable structure, efficient and durable catalytic performance, anti-interference ability and low ion leaching level, which provides a new idea for preparing heterogeneous catalyst to activate PMS to treat pharmaceutical wastewater, and has broad practical application prospects.

Biochar is widely recognized as an effective approach for mitigating heavy metal pollution. However, the utilization of machine learning models to guide biochar preparation and enhance its adsorption performance poses challenges. This study proposed a biochar design strategy guided by the Bayesian optimization algorithm. The strategy involves automated hyperparameter optimization for machine learning model training and exploration of unexplored biochar preparation conditions using the Bayesian algorithm. By leveraging Bayesian algorithms for hyperparameter search, we successfully crafted random forest models, support vector regression models, and back propagation models. In comparison to the previously reported models, these models demonstrated outstanding performance, with the random forest model in particular showcasing superior results (R2 = 0.998; RMSE = 0.027). Using a Bayesian algorithm, it was found that more than 80% of the feature combinations would exceed the upper limit of heavy metal adsorption. Our model revealed that biochar with a mesoporous structure, produced at a pyrolysis temperature of 420 °C, exhibited enhanced heavy metal adsorption capacity. This study presented a novel approach for the rapid development of machine learning models using Bayesian optimization and employed inverse reasoning to guide biochar preparation and enhance adsorption performance.

It has been a common way to recycle digestate after biogas production as a biofertilizer. However, the huge generation of digestate especially its liquid part surpasses the market consumption quantity, which in turn hinders the sustainable operation of a biogas plant. Biotreatment of liquid digestate (LD) with microorganisms is one way to reduce chemical oxygen demand (COD) and nitrogen content. This study enriched three microflorae from environmental water, liquid and solid digestate. After community structure analysis, the microflora from LD itself exhibits superior nitrogen removal function to the other two microflorae, and its predominant microbial strains are from Aliidiomarina, followed by Parapedobacter. The microflorae can grow at pH range from 7 to 10. pH and ammonium concentration show synergistic effect on the growth of microflorae. The microflora from LD can completely realize nitrogen removal in man-made medium within 48 h, and remove 93.7% ammonia nitrogen (NH3-N) and 88.1% COD from LD at optimum C/N ratio of 9. Sodium acetate and the fermented mash from grain ethanol production process are the preferable carbon sources to improve the removal of nitrogen and COD. The re-inoculation of indigenous microflora into LD can realize 2.9%~10.9% increase of NH3-N removal with or without addition of carbon sources, and 0.1%~11.7% improvement on COD removal with addition of carbon sources except glycerol. It means that the enrichment of the indigenous microflora combined with the addition of proper carbon source is a potential way to enhance the nitrogen and COD removal from LD.

This study investigates supercritical CO2 extraction of neutral lipids from Chlorella vulgaris NIES 227 microalgae, for biodiesel applications. While microalgae feedstocks are typically desiccated before extraction, drying is energy intensive and supercritical extraction from wet microalgae would be beneficial in reducing overall energy costs. The effects on the supercritical extraction kinetics, yields and extract composition of the water content of the initial biomass (either 0 or 27 wt.%), and of the operating pressure (200 and 250 bar) and temperature (40 and 60°C) were investigated. The highest total extraction yield (16.16 wt.% extract/dry biomass) was obtained with freeze-dried microalgae at 40°C and 200 bar. However, the extracts obtained at 40°C and 250 bar were the richest in fatty acids (0.96 g FA/extract), and the extracts obtained at 60°C and 250 bar had the highest cetane number (69) and oxidative stability (18 h). Water in the initial biomass had a negative impact on total extraction yields (3.89 wt.% extract/dry biomass at 200 bar and 40°C) and led to increased pigment extraction, but results suggest the presence of water may promote the extraction of fatty acids, in particular monounsaturated ones, highly desirable for biodiesel. In comparison, Soxhlet extraction with hexane was found to have higher lipid yields (31.20 wt.% extract/dry biomass) than any of the tested supercritical conditions, but more pigments were also extracted alongside, having a negative impact on oxidative stability. All the extracts obtained with supercritical CO2 and Soxhlet hexane met biofuel European standards for density, cetane numbers and iodine values.

Sulfur is a harmful impurity in iron ore, which seriously affects the subsequent smelting process and product quality. In this study, a novel process of hydrogen-based mineral phase transformation followed by magnetic separation was proposed to treat sulfur-bearing refractory iron ore. The results of pilot-scale experiments showed that in the oxidation heating stage, the sulfur element in the ore was oxidized to form SO2. During the reduction roasting stage, the hematite within iron ore powder was almost entirely transformed into magnetite at a reduction temperature of 520 °C using a gas combination of 45% H2- 15% CO- 40% N2, which significantly enhanced the magnetism of the particles. At this time, iron minerals could be effectively recovered by a grinding and low-intensity magnetic separation process. Under the optimum roasting and magnetic separation conditions, the iron grade of magnetic concentrate reached 66.40%, the iron recovery was 92.44%, and the sulfur content decreased significantly from 0.547% to 0.038%. The hydrogen-based mineral phase transformation technology showed unique technical advantages and environmental potential in treating sulfur-bearing refractory iron ores.

Tire wear microplastics (TWM) are formed by friction between tires and road surfaces during driving and they belong among the most abundant microplastics in the environment. However, the information about their fate in the environment is still unknown. The aim of this study was to investigate the aging of TWM in freshwater under controlled laboratory conditions over 12 weeks. The development of biofilm, changes in physical properties and chemical composition, leaching and biodegradation of TWM were followed. The results showed colonization of the TWM surface by microorganisms (up to 45 mg/g), which, however, began to detach from the particles after eight weeks, reducing the amount of biofilm. TWM initially leached zinc and organic compounds (expressed as dissolved organic carbon - DOC), but their concentrations were low and decreased with time. The increase in DOC was observed after 10 weeks, possibly due to the decomposition of the biofilm and the release of organic matter. Aging resulted in changes of density of TWM, but the morphology and chemical composition of the TWM surface did not change. This confirms the results of the biodegradability tests, which showed no biodegradation within 12 weeks. Overall, the results indicated that TWM are not readily biodegradable and therefore may accumulate and persist in the aquatic environment.

Lignin is a renewable natural resource that could be derived from oil palm empty fruit bunches. It has generated significant interest as a precursor in synthesizing graphene as anode and cathode material for supercapacitors. In this paper, we report the synthesis of 3D hierarchical Laser Scribed Graphene (LSG) on a flexible polyimide substrate from lignin extracted from empty fruit bunches (EFB) of oil palm for microsupercapacitor applications. The intensity and speed of the laser have been tuned to yield densely compacted oil palm lignin LSG at a laser power of 70% and a speed of 30% (OPL-LSG 7030). OPL-LSG 7030 possessed lower equivalent series resistance of 60.1 Ω and a larger crystalline size of ~31 nm than the rest of the tested samples. It exhibited exceptional areal capacitance of 30.77 mFcm-2 at a current density of 0.08 mAcm-2, an energy density of 0.00176 mWhcm-2 and a power density of 0.25 mWcm-2 when using a unique neutral PAAS/K2SO4 gel electrolyte. It achieved excellent capacitance retention of 88.4% after 5000 charge/discharge cycles and remarkable mechanical stability of 95% after 400 bending cycles. Furthermore, electrochemical studies revealed the redox properties of readily available quinone/ hydroquinone in the oil palm lignin, which could be inherited in graphene electrodes through a feasible and affordable approach for flexible green energy storage applications.

Al3+ generated during aluminum mining, electrolytic industry, and aluminum-based coagulant production enters sewage treatment plants and interacts with activated sludge, interfering with microbial growth and community succession. An anaerobic-anoxic-oxic (A2O) process was used to investigate the effect of Al3+ on biological denitrification, the metal form, and the microbial community structure. The results showed that a low concentration of Al3+ improved removal efficiencies of chemical oxygen demand (COD) and total nitrogen (TN) as well as biological activity. However, a high concentration of Al3+ reduced the COD and TN removal efficiencies. The removal efficiencies of COD, TN, and NH4+-N were the highest, and the INT-ETS values in the anaerobic, anoxic, and oxic zones were 93.21, 91.36, and 94.44 mg·INTF/(g·TSS·h) in the 10 mg/L Al3+ concentration treatment. Regardless of the change in Al3+ concentration, aluminum in the sludge mainly existed in the form of stable organic aluminum. Microbial richness and diversity decreased under the high concentration of Al3+. However, the relative abundance of Bacteroidetes and Chitinophagales increased, which was coincident with the change in microbial aluminum tolerance capacity. The dominant flora included Proteobacteria, Gammaproteobacteria, Betaproteobacteriales, Rhodocyclaceae, and Thauera. Amino acid and carbohydrate metabolism, as well as membrane transport and replication and repair, were the main metabolic pathways. K03088, K03406, and K02014 exhibited good adaptability under the high Al3+ concentration, which ensured effective removal of COD and TN.

This study addresses the gap in understanding of fabrication solvent influence on Cu-Co catalyst performance for MNZ degradation. By synthesizing recyclable Cu-Co catalysts using the co-precipitation method, the study investigates the impact of ethylene glycol (EG) solvent compared to conventional water (H2O) solvent. The optimized operational parameters resulted in stable and high MNZ degradation efficiency (above 90% removal) with twice-feeding of 1600 ppm H2O2, pH ~7.15, and 50 oC. The use of EG solvent enhances catalyst surface area, exposing more active sites with higher Cu+ and Cu2+ content, which incorporated in CoO6 environment with promoted redox property to facilitate H2O2 reaction and •OH production. This research contributes valuable insights into catalyst design and optimization, highlighting the potential of EG solvent for industrial application in antibiotic organic pollutant remediation.

As reported herein, we have designed an effective way to achieve in-situ loading of metal-organic frameworks (MOFs) into the pores of activated γ-Al2O3 particles to prepare low-cost, easy-to-obtain and high-yield granular MOFs composites (GMCs). MOF-5, ZIF-8, Ni-BTC, and Co-BTC have been selected to prepare GMCs via in-situ synthesis methods, thereby leading to the GMCs MOF-5-X@γ-Al2O3, ZIF-8-X@γ-Al2O3, Ni-BTC-X@γ-Al2O3, and Co-BTC-X@γ-Al2O3 (X = NO3 or OAc), respectively. The physical and chemical properties of the as-prepared MOF@γ-Al2O3 GMCs were characterized in detail. The results show that MOF-5-X@γ-Al2O3 and ZIF-8-X@γ-Al2O3 exhibit selective adsorption behavior for anionic dye. The adsorption capacities of MOF-5-X@γ-Al2O3 are 1388.01 mg g-1 (for CR and X = NO3), 1431.25 mg g-1 (for CR and X = OAc), 406.50 mg g-1 (for MO and X = NO3), and 234.16 mg g-1 (for MO and X = OAc), respectively, while the adsorption capacities of ZIF-8-X@γ-Al2O3 are 1426.85 mg g-1 (for CR and X = NO3), 1543.91 mg g-1 (for CR and X = OAc), 477.03 mg g-1 (for MO and X = NO3), and 451.02 mg g-1 (for MO and X = OAc), respectively. Moreover, ZIF-8-X@γ-Al2O3 has high adsorption performance for iodine molecules in solution, and the adsorption capacity reaches 630.63 mg g-1 for ZIF-8-NO3@γ-Al2O3 and 583.92 mg g-1 for ZIF-8-OAc@γ-Al2O3, respectively. This method is universal and can be used as an effective approach to prepare GMCs. In addition, the materials prepared by this method can be widely used in the adsorption of small molecules.

Heterogenous photocatalysis is a suitable technology for the removal of contaminants of emerging concern (CEC), such as parabens, from wastewaters. However, typically the photocatalyst is applied as a powder, which requires time-consuming and expensive supplementary separation processes, for its separation and recovery. Therefore, supported-photocatalysis has gained interest in the scientific community. To develop a suitable supported photocatalyst, commercial TiO2 (P25) powder was immobilized in polydimethylsiloxane (PDMS) membranes, to promote the degradation of three parabens (methylparaben -MP, ethylparaben -EP, and propylparaben -PP), under UV irradiation. To enhance the photocatalytic activity of the membranes, a plasma process was applied during their preparation. The plasma process operating conditions were optimized, regarding the working gas, the power applied, the pressure used and the processing time selected. Thus, the best conditions, among those analyzed, were the use of argon as the working gas, a power of 100 W, a pressure of 0.6 mbar and an operating time of 4 min. To assess the photocatalytic activity, two protocols, which varied in the P25 immobilization methodology (surface or matrix), were developed. It was concluded that PDMS membranes with P25 on the surface achieved higher removals of parabens during the photocatalytic oxidation and, when the preparation parameters were optimized, these membranes achieved removals of 53±2%, 53±0%, 58±2% for EP, MP and PP, respectively. As such, in this study, it was possible to develop a protocol to produce hydrophilic and photocatalytic P25/PDMS membranes efficient in the abatement of parabens under UV irradiation.

The imperative to establish environmentally friendly and sustainable food processing techniques has compelled the food industry to explore alternative approaches that uphold food quality, ensure nutritional integrity, and minimize energy consumption. Extensive research conducted in the past decade has substantiated the superiority of membrane-based dewatering technology over conventional methods, owing to its ability to retain nutrients effectively while minimizing energy requirements. Notably, forward osmosis (FO) and membrane distillation (MD) have emerged as viable membrane technologies for food processing in the industry. However, recent reviews have underscored the prominence of FO in the enrichment of liquid food, positioning it as a preferred choice among other membrane-based processes. This review paper aims to elucidate the advancements and contributions of FO and MD in the realm of food processing while evaluating their maturity and technology readiness level for food concentration. Moreover, it endeavors to delineate specific parameters, including pretreatment techniques, membrane cleaning strategies, and membrane configurations/modules tailored to liquid food sources' distinct dewatering requirements. Although most FO and MD studies have focused on lab-scale fruit juice and whey concentration, future investigations should encompass pilot-scale process development alongside comprehensive techno-economic analyses to facilitate the smooth transition of these technologies to an industrial scale.

Polyethylene terephthalate (PET) is a thermoplastic polymer which is the most used polyester in the plastics industry in the present day. It is predominately used to construct clothes fibres and food containers due to its properties.The problems surrounding this phenomenon are the basis for the decision to produce this plant facility. An alternative method of recycling PET is to perform a chemical reaction. Eight initial reaction routes were identified and narrowed down to three final processes according to their economic viability and sustainability: methanolysis, glycolysis and hydrolysis. These three processes were evaluated using the Triple Bottom Line (TBL) method by considering the effect each reaction has on the local community, environment, and economic potential. It was identified that glycolysis was the most suitable process due to its significant initial economic potential of 21.15M$/year calculated from the product and raw material costs. The reaction routes available for this process were researched and a final route was decided based on the operation costs and sustainability opportunities that the individual units offer.At the end of the economic evaluation for the process, it is determined that a profit value of 13.24M$/year can be obtained with a post-tax profit of 6.35M$/year. The equipment cost is evaluated as $6.63M with employability of 28 people. The start-up cost for the process will be $2.4M with a return on investment of 36% and a payback time of 3.5 years.

Thin-film composite membranes are vastly utilized to treat wastewater due to their high energy efficiency, low investment and environmental benignity. However, the use of hazardous solvents and non-renewable resources during membrane preparation poses a major threat to human health and the environment. Several tough challenges such as the trade-off effect between permeability and rejection as well as fouling require immediate remediation. To address these issues, this work integrated a green solvent and a bio-monomer, fructose in the membrane substrate and selective layer, respectively. The membrane is fabricated via facile interfacial polymerization with the addition of a zwitterionic monomer, 1-(2-hydroxyethyl) piperazine propane sulfonate (HEPPS) to promote antifouling properties. FTIR and XPS results depicted the formation of a polyesteramide membrane and the incorporation of zwitterion while AFM and FESEM micrographs showed the changes in membrane roughness. The synergistic effect of fructose and HEPPS in the selective layer increased water permeability from 3.54 to 4.77 L m-2 h-1 bar-1 while having a remarkable Na2SO4 rejection of 99.1%. Additionally, the zwitterionic membrane exhibited superior antifouling properties with a flux recovery ratio of 97.7% and 93.4% for bovine serum albumin and lysozyme, respectively. The results suggested that HEPPS and fructose could ameliorate the fouling resistance of the membrane significantly owing to their exceptional hydrophilicity. Moreover, the resultant membrane shows a stable chlorine resistance towards a high concentration of chlorine (10,000 ppm·h). The findings are expected to provide insights in designing membranes with improved antifouling properties and excellent separation performance coupled with green and sustainable fabrication.

Reasonably utilize the recyclable waste cardboard (175 million tons every year) had attracted the increasing environmental concern. However, the poor hydrophobicity and the loose porous structure of the cardboard-derived coating materials caused the rapid release of nutrients, thereby limiting the development and application of the bio-derived synthetic polymer coated controlled-release fertilizers (BPCFs). In this work, the hydrophobic-densified double-modified waste-carton-derived controlled-release fertilizers (HDCFs) were developed with nontoxic modifying agent and the simple production technology. The controlled release abilities of HDCFs were significantly enhanced (< 2 h to 120.45 days) and the nutrient release prediction models were established. The enhanced performance was attributed to the improved hydrophobicity and the obviously compact coating structure characterized by the three-dimensional computerized tomography (5.76 to 1.08%). Furthermore, the enhanced elasticity (5025.52 to 1325.68 MPa) of the HDCFs coatings also contributed to improve the controlled-release abilities. The controlled-release mechanism was also clarified: the atmosphere “stopper” in the “smaller and less” micropores in HDCFs coating only allows water vapor molecules (instead of liquid) slowly permeate into the internal urea core and significantly enhance the controlled-release longevities. The dramatically increased oilseed rape yield (71.75%) showed the efficient application effect of the HDCFs. All the results indicate that HDCF with 90:10 of the proportion of the castor oil and liquefaction polyhydric alcohols from cardboard (LPAC) and 5% of the siloxane of the total polyols exhibits the best performance effect. This work provides the efficient strategy to foster the end-user confidence in the low-cost and eco-friendly biowaste-derived controlled-release fertilizers.