Interfacial Mo-S-C Bond with High Reversibility for Advanced Alkali-Ion Capacitors: Strategies for High-Throughput Production.

The high-throughput scalable production of low-cost and high-performance electrode materials that work well under high power densities required in industrial application is full of challenges for the large-scale implementation of electrochemical technologies. Here, motivated by theoretical calculation that Mo-S-C heterojunction and sulfur vacancies can reduce the energy band gap, decrease the migration energy barrier, and improve the mechanical stability of MoS2 , the scalable preparation of inexpensive MoS2-x @CN is contrived by employing natural molybdenite as precursor, which is characteristic of high efficiency in synthesis process and energy conservation and the calculated costs are four orders of magnitude lower than MoS2 /C in previous work. More importantly, MoS2- x @CN electrode is endowed with impressive rate capability even at 5 A g-1 , and ultrastable cycling stability during almost 5000 cycles, which far outperform chemosynthesis MoS2 materials. Obtaining the full SIC cell assembled by MoS2- x @CN anode and carbon cathode, the energy/power output is high up to 265.3 W h kg-1 at 250 W kg-1 . These advantages indicate the huge potentials of the designed MoS2- x @CN and of mineral-based cost-effective and abundant resources as anode materials in high-performance AICs.

Bi2O3/BiO2 Nanoheterojunction for Highly Efficient Electrocatalytic CO2 Reduction to Formate.

Heterostructure engineering plays a vital role in regulating the material interface, thus boosting the electron transportation pathway in advanced catalysis. Herein, a novel Bi2O3/BiO2 heterojunction catalyst was synthesized via a molten alkali-assisted dealumination strategy and exhibited rich structural dynamics for an electrocatalytic CO2 reduction reaction (ECO2RR). By coupling in situ X-ray diffraction and Raman spectroscopy measurements, we found that the as-synthesized Bi2O3/BiO2 heterostructure can be transformed into a novel Bi/BiO2 Mott-Schottky heterostructure, leading to enhanced adsorption performance for CO2 and *OCHO intermediates. Consequently, high selectivity toward formate larger than 95% was rendered in a wide potential window along with an optimum partial current density of -111.42 mA cm-2 that benchmarked with the state-of-the-art Bi-based ECO2RR catalysts. This work reports the construction and fruitful structural dynamic insights of a novel heterojunction electrocatalyst for ECO2RR, which paves the way for the rational design of efficient heterojunction electrocatalysts for ECO2RR and beyond.

Efficient removal of NaOl from mineral processing wastewater using Al-electrocoagulation.

Sodium oleate (NaOl) is widely used as collector for oxidised ore flotation, and residual NaOl in mineral processing wastewater is a serious threat to mine environment. In this work, the feasibility of electrocoagulation (EC) as an alternative for chemical oxygen demand (COD) removal from NaOl-containing wastewater was demonstrated. Major variables were evaluated to optimise EC, and related mechanisms were proposed to interpret the observations in EC experiments. The initial pH of the wastewater greatly affected the COD removal efficiency, which was likely to be related to the variation of predominant species. When the pH was below 8.93 (original pH), liquid HOl(l) was the predominant specie, which could be rapidly removed by EC thought charge neutralisation and adsorption. At original pH or higher, Ol- could react with dissolved Al3+ to form insoluble Al(Ol)3, which was subsequently removed through charge neutralisation and adsorption. The presence of fine mineral particles could reduce repulsion force of the suspended solids and promote flocculation, whereas the presence of water glass had an opposite effect. These results demonstrated that EC can be employed as an effective process to purify NaOl-containing wastewater. This study will contribute to deepening our understanding of EC technology for NaOl removal and provide useful information to researchers in mineral processing industry.

Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane.

Highly selective photoreduction of CO2 to valuable hydrocarbons is of great importance to achieving a carbon-neutral society. Precisely manipulating the formation of the Metal1 ⋅⋅⋅C=O⋅⋅⋅Metal2 (M1 ⋅⋅⋅C=O⋅⋅⋅M2 ) intermediate on the photocatalyst interface is the most critical step for regulating selectivity, while still a significant challenge. Herein, inspired by the polar electronic structure feature of CO2 molecule, we propose a strategy whereby the Lewis acid-base dual sites confined in a bimetallic catalyst surface are conducive to forming a M1 ⋅⋅⋅C=O⋅⋅⋅M2 intermediate precisely, which can promote selectivity to hydrocarbon formation. Employing the Ag2 Cu2 O3 nanowires with abundant Cu⋅⋅⋅Ag Lewis acid-base dual sites on the preferred exposed {110} surface as a model catalyst, 100 % selectivity toward photoreduction of CO2 into CH4 has been achieved. Subsequent surface-quenching experiments and density functional theory (DFT) calculations verify that the Cu⋅⋅⋅Ag Lewis acid-base dual sites do play a vital role in regulating the M1 ⋅⋅⋅C=O⋅⋅⋅M2 intermediate formation that is considered to be prone to convert CO2 into hydrocarbons. This study reports a highly selective CO2 photocatalyst, which was designed on the basis of a newly proposed theory for precise regulation of reaction intermediates. Our findings will stimulate further research on dual-site catalyst design for CO2 reduction to hydrocarbons.

Molecular Dynamics Beyond the Monolayer Adsorption as Derived from Langmuir Curve Fitting.

Langmuir adsorption model is a classic physical-chemical adsorption model and is widely used to describe the monolayer adsorption behavior at the material interface in environmental chemistry. Traditional adsorption dynamic modeling solely considered the surface physiochemical interaction between the adsorbent and adsorbate. The surface reaction dynamics resulting from the heterogeneous surface and intrinsic electronic structure of absorbents were rarely considered within the reported adsorption experiments. Herein, by employing the chlorine hybrid graphene oxide (GO-Cl) to adsorb Ag+ in an aqueous solution, complicated molecular dynamics significantly deviated from the monolayer adsorption mechanism, as suggested by Langmuir adsorption curve fitting, has been elucidated down to atomic scale. In the time-dependent Ag adsorption experiments, both Ag single atoms and Ag/AgCl nanoparticle heterostructures are observed to be formed sequentially on GO-Cl. These observations indicate that for the surface adsorption dynamics, not only the surface chemical adsorption process involved but also photoreduction and the C-Cl bond cleavage reaction has been heavily engaged within the GO-Cl interface, suggesting a much more complicated vision rather than the monolayered adsorption algorithm as derived from curve fitting. This study uses GO-Cl as a simple example to disclose the complicated adsorption dynamic process underneath Langmuir adsorption curve fitting. It advocates the necessity of imaging the interfacial atomic-scale dynamic structure with high-resolution microscopy techniques in modern adsorption studies, rather than simply explaining the adsorption dynamics relying on the curve fitting results due to the complicated physiochemical reactivity of the adsorbents.

Electrochemical Driven Phase Segregation Enabled Dual-Ion Removal Battery Deionization Electrode.

Battery deionization (BDI) offers a powerful platform for integrating water treatment and energy conversion. Exploring novel BDI electrode materials with high energy storage capacity and high efficiency for both cations and anions removal is the key to advancing the BDI technique. Herein, we report the first BDI electrode material capable of simultaneously removing Cl- (58.4 mg g-1) and Na+ (8.7 mg g-1) in water with a reversible capacity of 160 mAh g-1. In situ powder X-ray diffraction (PXRD) unravels that the dual-ion removal capability is attributed to a novel reversible electrochemical driven phase segregation reaction mechanism between NaBi3O4Cl2 and the in situ formed metallic Bi. The unique dual-ion storage capability demonstrated with the NaBi3O4Cl2 electrode indicates that exploring electrochemical reversible phase segregation electrode material holds great promise for advancing the BDI electrode for future desalination techniques and aqueous rechargeable battery systems.

Migration behavior of impurities during the purification of waste graphite powders.

Metal-laden solid wastes (e.g., waste graphite powders) have attracted great attention owing to their hazardous effects on the surrounding soil and water. Additionally, the metal-bearing impurities also hinder the reutilization of waste graphite powders. Thus, it is necessary to remove these inorganic impurities and figure out the removal mechanism of impurities in the purification process. In this study, an alkaline roasting-water washing-acid leaching (AWA) method was used to upgrade the waste graphite powders, and the migration behavior of diverse impurities has been qualitatively and quantitatively investigated. A graphite product with high impurity removal efficiencies is attained under optimal conditions. The removal of impurities mainly follows three routes: (1) V-, P-, and S-bearing impurities were complete removed (some formed soluble salts during alkaline roasting, and the remainder was dissolved in acid); (2) most Al-, K-, and Si-bearing impurities were removed by alkaline roasting, with the remainder was dissolved in the acid-leaching process; and (3) Fe-, Mg-, Ti-, Ca-, and Zn-bearing impurities were decomposed at high temperature and reacted with alkali to form hydroxides or oxides, which was subsequently dissolved in acid. In addition, the treatment of the generated wastewater is also discussed. The uncovered migration mechanisms of diverse impurities would guide the purification and reutilization process of other metal-bearing solid wastes efficiently.

Converting Spent LiFePO4 Battery into Zeolitic Phosphate for Highly Efficient Heavy Metal Adsorption.

Developing efficient recycling technologies for large-scale spent batteries is the key to build a zero-waste city. Herein, a [Al8.5Fe0.5P12O48]·[C24H72N16]·[Li·4H2O]·[12H2O] (AlFePO-Li) zeolite, crystallizing in space group I4̅3m with a = 16.6778(3) Å, has been constructed via the hydrothermal treatment of spent LiFePO4 battery. Benefiting from the three-dimensional 12-member-ring channels in its structure and chemical adsorption, excellent Pb2+ removal capacity up to 723.8 mg g-1 has been achieved. Detailed adsorption mechanism study revealed that the cation exchange capacity is significantly contributed by ion exchange of the protonated organic amine cations in the zeolite channel and the protons from the framework dangling phosphate group. This work demonstrates a novel method of reutilizing spent LIBs to construct zeolite for heavy metal removal. It is of great importance to achieve sustainable development based on the "resource utilization" and "trash-to-treasure" strategy.

Mixed Redox-Couple-Involved Chalcopyrite Phase CuFeS2 Quantum Dots for Highly Efficient Cr(VI) Removal.

Iron-based nanosized ecomaterials for efficient Cr(VI) removal are of great interest to environmental chemists. Herein, inspired by the "mixed redox-couple" cations involved in the crystal structure and the quantum confinement effects resulting from the particle size, a novel type of iron-based ecomaterial, semiconducting chalcopyrite quantum dots (QDs), was developed and used for Cr(VI) removal. A high removal capacity up to 720 mg/g was achieved under optimal pH conditions, which is superior to those of the state-of-the-art nanomaterials for Cr(VI) removal. The mechanism of Cr(VI) removal was elucidated down to an atomic scale by combining comprehensive characterization techniques with adsorption kinetic experiments and DFT calculations. The experimental results revealed that the material was a good electron donor semiconductor attributed to the existence of "mixed redox couple of Cu(I)-S-Fe(III)" in the crystal structure. With the size-dependent quantum confinement effect and the high surface area, the semiconducting chalcopyrite QDs could effectively remove Cr(VI) from aqueous solution through a syngenetic photocatalytic reduction and adsorption mechanism. This study not only reports the design histogram of the iron-based CuFeS2 QD ecomaterial for efficient Cr(VI) removal but also paves the way for understanding the atomic-scale mechanism behind the syngenetic effects of using the QD semiconducting material for Cr(VI) removal.

Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel.

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management. Recently, electrocatalytically converting polyethylene terephthalate (PET) into formate and hydrogen has aroused great interest, while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol (PET monomer) oxidation reaction (EGOR) remains a challenge. Herein, a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy. Benefiting from the interconnected ultrathin nanosheet architecture, dual dopants induced up-shifting d band centre and facilitated in situ structural reconstruction, the Co and Cl co-doped Ni3S2 (Co, Cl-NiS) outperforms the single-doped and undoped analogues for EGOR. The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency (> 92%) and selectivity (> 91%) at high current densities (> 400 mA cm-2). Besides producing formate, the bifunctional Co, Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h-1 in 2 M KOH, at 1.7 V. This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes, but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

Interfacial Coordination Bonding-Assisted Redox Mechanism-Driven Highly Selective Precious Metal Recovery on Covalent-Functionalized Ultrathin 1T-MoS2.

Rational design of functional material interfaces with well-defined physico-chemical-driven forces is crucial for achieving highly efficient interfacial chemical reaction dynamics for resource recovery. Herein, via an interfacial structure engineering strategy, precious metal (PM) coordination-active pyridine groups have been successfully covalently integrated into ultrathin 1T-MoS2 (Py-MoS2). The constructed Py-MoS2 shows highly selective interfacial coordination bonding-assisted redox (ICBAR) functionality toward PM recycling. Py-MoS2 shows state-of-the-art high recovery selectivity toward Au3+ and Pd4+ within 13 metal cation mixture solutions. The related recycling capacity reaches up to 3343.00 and 2330.74 mg/g for Au3+ and Pd4+, respectively. More importantly, above 90% recovery efficiencies have been achieved in representative PMs containing electronic solid waste leachate, such as computer processing units (CPU) and spent catalysts. The ICBAR mechanism developed here paves the way for interface engineering of the well-documented functional materials toward highly efficient PM recovery.

Waste-Derived Catalysts for Water Electrolysis: Circular Economy-Driven Sustainable Green Hydrogen Energy.

The sustainable production of green hydrogen via water electrolysis necessitates cost-effective electrocatalysts. By following the circular economy principle, the utilization of waste-derived catalysts significantly promotes the sustainable development of green hydrogen energy. Currently, diverse waste-derived catalysts have exhibited excellent catalytic performance toward hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and overall water electrolysis (OWE). Herein, we systematically examine recent achievements in waste-derived electrocatalysts for water electrolysis. The general principles of water electrolysis and design principles of efficient electrocatalysts are discussed, followed by the illustration of current strategies for transforming wastes into electrocatalysts. Then, applications of waste-derived catalysts (i.e., carbon-based catalysts, transitional metal-based catalysts, and carbon-based heterostructure catalysts) in HER, OER, and OWE are reviewed successively. An emphasis is put on correlating the catalysts' structure-performance relationship. Also, challenges and research directions in this booming field are finally highlighted. This review would provide useful insights into the design, synthesis, and applications of waste-derived electrocatalysts, and thus accelerate the development of the circular economy-driven green hydrogen energy scheme.

Unlocking bimetallic active sites via a desalination strategy for photocatalytic reduction of atmospheric carbon dioxide.

Ultrathin two-dimensional (2D) metal oxyhalides exhibit outstanding photocatalytic properties with unique electronic and interfacial structures. Compared with monometallic oxyhalides, bimetallic oxyhalides are less explored. In this work, we have developed a novel top-down wet-chemistry desalination approach to remove the alkali-halide salt layer within the complicated precursor bulk structural matrix Pb0.6Bi1.4Cs0.6O2Cl2, and successfully fabricate a new 2D ultrathin bimetallic oxyhalide Pb0.6Bi1.4O2Cl1.4. The unlocked larger surface area, rich bimetallic active sites, and faster carrier dynamics within Pb0.6Bi1.4O2Cl1.4 layers significantly enhance the photocatalytic efficiency for atmospheric CO2 reduction. It outperforms the corresponding parental matrix phase and other state-of-the-art bismuth-based monometallic oxyhalides photocatalysts. This work reports a top-down desalination strategy to engineering ultrathin bimetallic 2D material for photocatalytic atmospheric CO2 reduction, which sheds light on further constructing other ultrathin 2D catalysts for environmental and energy applications from similar complicate structure matrixes.

Transferring waste red mud into ferric oxide decorated ANA-type zeolite for multiple heavy metals polluted soil remediation.

Herein, a novel "waste reclamation for soil remediation" strategy has been developed for both alkaline waste red mud (RM) recycling and heavy metal (HM) polluted soil remediation. Through a direct one-pot hydrothermal reaction process, the Al, Si, alkali, and Fe2O3 components in waste RM have been transferred into ferric oxide decorated ANA-type zeolite (Fe2O3-ANA). As tested by the HMs polluted soil remediation and oilseed rape planting experiment, when 25 g/kg Fe2O3-ANA is added into the Pb2+, Cu2+, Cr3+ and anionic AsO2- polluted soil (HM concentration: 100-200 mg/kg), it can effectively suppress the HMs mobility in soil and reduce the bio-accumulation concentrations of HMs in the harvested oilseed rape (reduce ratio: 37.9-69.5%). The detailed mechanism study using energy dispersive X-ray energy spectroscopy, in-depth X-ray photoelectron spectroscopy and density function theory calculation concludes that the Cu2+, Pb2+ and Cr3+ in soil have been adsorbed and trapped in the framework structure of ANA in Fe2O3-ANA mainly via the cation exchange process. While the anionic AsO2- species are mainly caught by the Fe2O3 component in Fe2O3-ANA via surface adsorption. Overall, this work firstly transforms waste RM into Fe2O3-ANA for soil remediation, which is valuable to waste resource recycling and environmental conservation.

Enhanced Cr(VI) reduction on natural chalcopyrite mineral modulated by degradation intermediates of RhB.

Wastewater with complex compositions of both heavy metals and organic pollutants is of critical environmental and socioeconomic threat worldwide, which urgently requires feasible remediation technologies to target this challenge. In this study, natural chalcopyrite (CuFeS2, NCP), the most abundant copper-based mineral in the Earth's crust, has been discovered to be a heterogeneous catalyst that can activate peroxydisulfate (PDS) for the simultaneous degradation of organic pollutant Rhodamine B (RhB) and reduction of hexavalent chromium (Cr(VI)). Batch experimental results indicate that both RhB and Cr(VI) could be simultaneously removed under a near-neutral condition in NCP/PDS combined system. The radicals SO4•- and •OH generated from PDS activation are the main oxidative species detected by electron paramagnetic resonance (EPR) spectroscopy. SO4•- acted as a predominant role in RhB degradation, while Cr(VI) reduction is mainly attributed to the oxidization of S2- and S22- species on NCP surface, as well as the photoreduction performance of NCP, which could be enhanced by the intermediates generated from RhB degradation. Density functional theory (DFT) calculation results disclose that Fe is the critical catalytic site for PDS activation. This work demonstrates a user-friendly strategy for remediation of complex wastewater containing both heavy metal and organic pollutants by combining photoreduction and advanced oxidation processes (AOPs) with natural minerals. It paves a way for wastewater treatment by utilizing low-cost natural abundant minerals as catalysts.

Interfacial engineering of CuFeS2 quantum dots via platinum decoration with enhanced Cr(VI) reduction dynamics under UV-Vis-NIR radiation.

Configuring reactive and stable catalytic interfaces is crucial to design efficient photocatalysts for Cr(VI) reduction. Herein, via the platinum decoration approach based on interfacial engineering, we developed an effective catalytic interface within novel semiconducting chalcopyrite quantum dots (Pt/CuFeS2 QDs). Benefiting from the catalytic merits of the Pt modulated interfacial structure and electronic structure, Pt/CuFeS2 QDs show a broader light absorption capability extending to near-infrared radiation (NIR) range with superior carriers separation performance and faster charge transfer efficiency, which delivers a three-folder faster photocatalytic Cr(VI) reduction efficiency comparing to the original CuFeS2 QDs. Density functional theory (DFT) calculations unravel that Pt atoms prefer to be anchored with the surface S atoms to form a stable interfacial structure with faster electron transfer and Cr(VI) reduction dynamics. This work demonstrates that platinum decoration based on interfacial engineering is an effective strategy to simultaneously modulate the band structure and accelerate the interfacial reaction dynamics for semiconductor photocatalysts, which paves the way for designing highly efficient photocatalysts for light-driven environmental and energy engineering applications.

NiCoSx@Cobalt Carbonate Hydroxide Obtained by Surface Sulfurization for Efficient and Stable Hydrogen Evolution at Large Current Densities.

Developing earth-abundant, active, and stable electrocatalysts for hydrogen evolution reactions (HERs) at large current densities has remained challenging. Herein, heterostructured nickel foam-supported cobalt carbonate hydroxide nanoarrays embellished with NiCoSx nanoflakes (NiCoSx@CoCH NAs/NF) are designed via room-temperature sulfurization, which can drive 10 and 1000 mA cm-2 at low overpotentials of 55 and 438 mV for HER and exhibit impressive long-term stability at the industrial-level current density. Surprisingly, NiCoSx@CoCH NAs/NF after a 500 h stability test at 500 mA cm-2 exhibit better catalytic performance than the initial one at high current densities. Simulations showed that NiCoSx@CoCH NAs have an optimized hydrogen adsorption free energy (ΔGH*) of 0.02 eV, owing to the synergistic effect of CoCH (ΔGH* = 1.36 eV) and NiCoSx (ΔGH* = 0.03 eV). The electric field at the heterostructure interface leads to electron transport from CoCH to NiCoSx, which enhances HER dynamics. The hierarchical nanostructure has a large specific area and a superaerophobic surface, which are beneficial to hydrogen generation/release for efficient and stable HER.

Converting loess into zeolite for heavy metal polluted soil remediation based on "soil for soil-remediation" strategy.

Both soil erosion and soil contamination pose critical environmental threats to the Chinese Loess Plateau (CLP). Green, efficient and feasible remediation technologies are highly demanded to meet these challenges. Herein we propose a unique "soil for soil-remediation" strategy to remediate the heavy metal polluted soil in CLP by converting loess into zeolite for the first time. With a simple template-free route, the natural loess can be converted into cancrinite (CAN) type of zeolite. A highly crystalline CAN was obtained via hydrothermal treatment at 240 oC for 48 h, with a precursor alkalinity of Na/(Si+Al)> 2.0. The as-synthesized CAN zeolite exhibits excellent remediation performance for Pb(II) and Cu(II) polluted soil. Plant assay experiment demonstrates that CAN can significantly restrain the uptake and accumulation of Pb(II) and Cu(II) ions in vegetables, with a high removal efficiency up to 90.7% and 81.4%, respectively. This work demonstrates a "soil for soil-remediation" strategy to utilize the natural loess for soil remediation in CLP, which paves the way for developing green and sustainable remediation eco-materials with local loess as raw materials.

Protonation stabilized high As/F mobility red mud for Pb/As polluted soil remediation.

The hazardous red mud (RM) with high As/F mobility and heavy metal contaminated soil have constituted severe environmental threats. This work demonstrates a "waste to eco-material" strategy through a reliable and low-cost protonation approach to eliminate the As/F leaching risk of RM, and then recycle it as heavy metal passivators for Pb/As polluted soil remediation. The As/F anions have been immobilized by the protonated Fe/Al (hydr)oxides within RM via the formation of stable As/F compounds during the protonation process, which satisfies the requirement by the World Health Organization (As leaching <0.01 mg/L; F leaching <0.8 mg/L). Moreover, in the oilseed rape pot experiments, by adding 30 g/kg stabilized RM into Pb/As polluted soils (100 ~ 300 ppm), benefited from its large adsorption capacity, approximately 40.9 ~ 49.7% Pb and 40.8 ~ 54.8% As concentrations in the plant are reduced without adverse effects. The whole process for RM treatment and soil remediation is cost-effective, straightforward and eco-friendly without secondary pollution or soil degradation. This research provides a green chemical strategy to address both RM recycling and heavy metal contaminated soil remediation problems, which shows high economic feasibility and ecological benefits.

Remediation of Cu-polluted soil with analcime synthesized from engineering abandoned soils through green chemistry approaches.

Due to the large output and potential ecological risks, disposal of engineering abandoned soils (EAS) has become an enormous challenge for human society. Herein, EAS has been transformed into microporous analcime (ANA) zeolite material through a fast, energy-efficient, and straightforward conversion process. The as-synthesized ANA has been employed to remediate Cu-polluted soil, which shows a significant ecological restoration function in a vegetable pot experiment. With 25 g/kg ANA into Cu contaminated soil (total Cu concentration: 200 ppm), the Cu accumulation concentration in vegetables has been decreased from 5.60 down to 1.80 mg/kg (approaching the background Cu level 1.70 mg/kg in vegetables). Detailed mechanism study combining with DFT calculations reveals that the Cu2+ in soil has been captured both inside the ANA pore channels and on the surface via ion-exchange and surface adsorption mechanism. The whole process, including ANA synthesis and Cu polluted soil remediation, has been optimized to show a valuable conceptual model to recycle EAS resource and in-situ remediate Cu polluted soil.