Scalable S/N Co-Functionalized Activated Carbon for Targeted Recovery of Multiple Precious Metals from Industrial Waste Streams

Hongjie Zhou; Xiaoqiang An; Tianshu Zhang; Mingran Li; Lingru Kong; Huachun Lan; Huijuan Liu; Jiuhui Qu

doi:10.1016/j.eng.2026.01.020

Engineering ›› :202601020 DOI: 10.1016/j.eng.2026.01.020

Research

research-article

Scalable S/N Co-Functionalized Activated Carbon for Targeted Recovery of Multiple Precious Metals from Industrial Waste Streams

Author information +

History +

PDF

Abstract

The recovery of precious metals (PMs) from industrial waste streams is constrained by the scarcity of adsorbents that reconcile scalable production, multi-metal selectivity, and cost-effectiveness. Here, we engineered S/N co-functionalized activated carbon to overcome these challenges by combining hierarchical porosity with an electron-enhanced surface of a multifunctional S/N network. The optimal S/N co-functionalized activated carbon (AC2) is synthesized via a scalable one-pot solvothermal method (92% yield, 0.532 kg·batch^-1), immobilizing thioamide, polysulfide, imine, and amine functionalities onto a micro-mesoporous carbon matrix. This design enables ultra-trace PM uptake (1 μg·L^-1) with exceptional residual levels (<0.001 μg·L^-1) and remarkable adsorption capacities (1750, 940, and 270 mg·g^-1 for Au, Pd, and Pt, respectively). Practical validation in e-waste and catalyst leachates (>96% recovery) and spiked surface water (92%-97% PM uptake with 10000 fold competing metal concentrations) demonstrates robust performance in real-world hydrometallurgical and ecological contexts. The adsorbent’s techno-economic viability is further underscored by acid-resistant reusability (>15 cycles), a 34 fold cost reduction at scale (370 CNY·kg^-1), and over 90% lower life cycle environmental impacts. This work establishes a paradigm for resource-efficient urban mining, integrating scalable material design with critical metal recovery to address global resource circularity challenges.

Keywords

S/N co-functionalization / Scalable synthesis / Precious metal recovery / Selective adsorption / Coordination-reduction / Urban mining

Cite this article

Download citation ▾

Hongjie Zhou, Xiaoqiang An, Tianshu Zhang, Mingran Li, Lingru Kong, Huachun Lan, Huijuan Liu, Jiuhui Qu. Scalable S/N Co-Functionalized Activated Carbon for Targeted Recovery of Multiple Precious Metals from Industrial Waste Streams. Engineering 202601020 DOI:10.1016/j.eng.2026.01.020

登录浏览全文

4963

注册一个新账户忘记密码

References

Publishing order | Descend order by publishing year | Descend order by cited within

[1]	Ahmad M, Shah T, Tariq MR, Zhang L, Lyu Y, Iqbal W, et al. Recent trends in material design and preparation with structure-activity relationship for gold recovery from e-waste: a review. J Clean Prod 2023;426:139012.

[2]	Zupanc A, Install J, Jereb M, Repo T. Sustainable and selective modern methods of noble metal recycling. Angew Chem Int Ed Engl 2023; 62(5):e202214453.

[3]	Taghvaie Nakhjiri A, Sanaeepur H, Ebadi Amooghin A, Shirazi MMA. Recovery of precious metals from industrial wastewater towards resource recovery and environmental sustainability: a critical review. Desalination 2022;527:115510.

[4]	Cheng YZ, Bao X, Jiang D, Ji W, Yang DH, Ding X, et al. Light-promoted extraction of precious metals using a porphyrin-integrated one-dimensional covalent organic framework. Angew Chem Int Ed Engl 2025; 64(2): e202414943.

[5]	Mei D, Yan B. A 2D acridine-based covalent organic framework for selective detection and efficient extraction of gold from complex aqueous-based matrices. Angew Chem Int Ed Engl 2024; 63(24):e202402205.

[6]	Bashri M, Kumar S, Bhandari P, Stephen S, O’Connor MJ, Gaber S, et al. Hydrazone-linked covalent organic framework catalyst via efficient Pd recovery from wastewater. ACS Appl Mater Interfaces 2025; 17(12):17804-12.

[7]	Jiang D, Wang ZL, Cheng YZ, Yu YX, Kong HY, Bian XY, et al. A sulfhydryl-functionalized vinylene-linked covalent organic framework for promoting gold recovery by light-assistance. Chem Eng J 2024;497:154212.

[8]	Wu Y, Zeng SH, Xu W, Chen YR, Liu K, Dai YT, et al. Thiophene-functionalized covalent triazine frameworks for photo-enhanced gold recovery. Separ Purif Tech 2024;345:127408.

[9]	Zhang L, Zheng QQ, Xiao SJ, Chen JQ, Jiang W, Cui WR, et al. Covalent organic frameworks constructed by flexible alkyl amines for efficient gold recovery from leaching solution of e-waste. Chem Eng J 2021;426:131865.

[10]	Chen S, Yang Y, Zi F, Hu X, Li X. Constructing phosphine-containing microspheres for selective recovery of gold(I) thiosulfate complex by adjusting the interaction site. Separ Purif Tech 2025;362:131636.

[11]	Mahandra H, Faraji F, Ghahreman A. Novel extraction process for gold recovery from thiosulfate solution using phosphonium ionic liquids. ACS Sustain Chem & Eng 2021; 9(24):8179-85.

[12]	Wang R, Zou H, Zheng R, Feng X, Xu J, Shangguan Y, et al. Molecular dynamics beyond the monolayer adsorption as derived from Langmuir curve fitting. Inorg Chem 2022; 61(20):7804-12.

[13]	Zuhra Z, Haris Khan M, Ali S, Ahmad M, Zhang Z. Metal-organic frameworks for sustainable precious metal recovery: a review of recent advances. Chem Eng J 2024;500:157105.

[14]	Guo W, Liu J, Tao H, Meng J, Yang J, Shuai Q, et al. Covalent organic framework nanoarchitectonics: recent advances for precious metal recovery. Adv Mater 2024; 36(33):2405399.

[15]	Wang K, Qiao X, Ren H, Chen Y, Zhang Z. Industrialization of covalent organic frameworks. J Am Chem Soc 2025; 147(10):8063-82.

[16]	Huang Y, Yu Y, Hu R, Tang BZ. Multicomponent polymerizations of elemental sulfur, CH₂Cl₂, and aromatic amines toward chemically recyclable functional aromatic polythioureas. J Am Chem Soc 2024; 146(21):14685-96.

[17]	Cao W, Dai F, Hu R, Tang BZ. Economic sulfur conversion to functional polythioamides through catalyst-free multicomponent polymerizations of sulfur, acids, and amines. J Am Chem Soc 2020; 142(2):978-86.

[18]	Wang R, Shangguan Y, Feng X, Gu X, Dai W, Yang S, et al. Interfacial coordinational bond triggered photoreduction membrane for continuous light-driven precious metals recovery. Nano Lett 2023; 23(6):2219-27.

[19]	Su Y, Berbille A, Li XF, Zhang J, PourhosseiniAsl M, Li H, et al. Reduction of precious metal ions in aqueous solutions by contact-electro-catalysis. Nat Commun 2024; 15(1):4196.

[20]	Kadivar S, Pourhossein F, Mousavi SM. Recovery of valuable metals from spent mobile phone printed circuit boards using biochar in indirect bioleaching. J Environ Manage 2021;280:111642.

[21]	Wang B, Lan J, Bo C, Gong B, Ou J. Adsorption of heavy metal onto biomass-derived activated carbon: review. RSC Adv 2023; 13(7):4275-302.

[22]	Chang Z, Zeng L, Sun C, Zhao P, Wang J, Zhang L, et al. Adsorptive recovery of precious metals from aqueous solution using nanomaterials—a critical review. Coord Chem Rev 2021;445:214072.

[23]	Wang C, Chen S, Chen Y, Zi F, Hu X, Qin X, et al. Modification of activated carbon by chemical vapour deposition through thermal decomposition of thiourea for enhanced adsorption of gold thiosulfate complex. Separ Purif Tech 2020;241:116632.

[24]	de la Torre-Miranda N, Reilly L, Eloy P, Poleunis C, Hermans S. Thiol functionalized activated carbon for gold thiosulfate recovery, an analysis of the interactions between gold and sulfur functions. Carbon 2023; 204: 254-67.

[25]	Zhang L, Li B, Shao P, Zhou X, Li D, Hu Z, et al. Selective capture of palladium from acid wastewater by thiazole-modified activated carbon: performance and mechanism. Environ Res 2023; 238(Pt 2):117253.

[26]	Chen Y, Zi F, Hu X, Yang P, Ma Y, Cheng H, et al. The use of new modified activated carbon in thiosulfate solution: a green gold recovery technology. Separ Purif Tech 2020;230:115834.

[27]	Eskandari P, Abousalman-Rezvani Z, Roghani-Mamaqani H, Salami-Kalajahi M. Polymer-functionalization of carbon nanotube by in situ conventional and controlled radical polymerizations. Adv Colloid Interface Sci 2021;294:102471.

[28]	Hu Y, Zhang L, Wang Z, Hu R, Tang BZ. Economical synthesis of functional aromatic polythioamides from KOH-assisted multicomponent polymerizations of sulfur, aromatic diamines and dialdehydes. Polym Chem 2023; 14(21):2617-23.

[29]	Hu Q, Lan R, He L, Liu H, Pei X. A critical review of adsorption isotherm models for aqueous contaminants: curve characteristics, site energy distribution and common controversies. J Environ Manage 2023;329:117104.

[30]	Xue T, He T, Peng L, Syzgantseva OA, Li R, Liu C, et al. A customized MOF-polymer composite for rapid gold extraction from water matrices. Sci Adv 2023; 9(13):eadg4923.

[31]	Vetere V, Adamo C, Maldivi P. Performance of the ‘parameter free’ PBE0 functional for the modeling of molecular properties of heavy metals. Chem Phys Lett 2000; 325(1-3):99-105.

[32]	Grimme S, Antony J, Ehrlich S, Krieg H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J Chem Phys 2010; 132(15):154104.

[33]	Grimme S, Ehrlich S, Goerigk L. Effect of the damping function in dispersion corrected density functional theory. J Comput Chem 2011; 32(7):1456-65.

[34]	Weigend F, Ahlrichs R. Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: design and assessment of accuracy. Phys Chem Chem Phys 2005; 7(18):3297-305.

[35]	Miertuš S, Scrocco E, Tomasi J. Electrostatic interaction of a solute with a continuum. A direct utilizaion of ab initio molecular potentials for the prevision of solvent effects. Chem Phys 1981; 55(1):117-29.

[36]	Schäfer A, Huber C, Ahlrichs R. Fully optimized contracted gaussian basis sets of triple zeta valence quality for atoms Li to Kr. J Chem Phys 1994; 100(8):5829-35.

[37]	Frisch MJ, Trucks GW, Schlegel HB, Scuseria GE, Robb MA, Cheeseman JR, et al. Gaussian 16 rev. C.01. Wallingford, CT: Gaussian Inc.; 2016.

[38]	Gao S, Chen X, Qu J, Guo Y, Shi H, Pang F, et al. Recycling of silicon solar panels through a salt-etching approach. Nat Sustain 2024;7(7):920-30.

[39]	Yue TJ, Ren WM, Lu XB. Copolymerization involving sulfur-containing monomers. Chem Rev 2023; 123(24):14038-83.

[40]	Zhao X, Gao P, Shen B, Wang X, Yue T, Han Z. Recent advances in lignin-derived mesoporous carbon based-on template methods. Renew Sustain Energy Rev 2023;188:113808.

[41]	Kale AD, Dalal DS. Catalyst-and solvent-free thioamidation of aromatic aldehydes through a Willgerodt-Kindler reaction. ChemistrySelect 2022; 7(48):e202203497.

[42]	Yao Z, Shao P, Fang D, Shao J, Li D, Liu L, et al. Thiol-rich, porous carbon for the efficient capture of silver: understanding the relationship between the surface groups and transformation pathways of silver. Chem Eng J 2022;427:131470.

[43]	Song KS, Ashirov T, Talapaneni SN, Clark AH, Yakimov AV, Nachtegaal M, et al. Porous polyisothiocyanurates for selective palladium recovery and heterogeneous catalysis. Chem 2022; 8(7):2043-59.

[44]	Jia H, Yao N, Jin Y, Wu L, Zhu J, Luo W. Stabilizing atomic Ru species in conjugated sp² carbon-linked covalent organic framework for acidic water oxidation. Nat Commun 2024; 15(1):5419.

[45]	Li G, Ye J, Fang Q, Liu F. Amide-based covalent organic frameworks materials for efficient and recyclable removal of heavy metal lead (II). Chem Eng J 2019;370:822-30.

[46]	MacDonald L, Zhang D, Karamalidis A. Platinum group metals: key solid phase adsorption technologies for separation from primary and secondary sources. Resour Conserv Recycling 2024;205:107590.

[47]	Shin SS, Jung Y, Jeon S, Park SJ, Yoon SJ, Jung KW, et al. Efficient recovery and recycling/upcycling of precious metals using hydrazide-functionalized star-shaped polymers. Nat Commun 2024; 15(1):3889.

[48]	Li F, Zhu J, Sun P, Zhang M, Li Z, Xu D, et al. Highly efficient and selective extraction of gold by reduced graphene oxide. Nat Commun 2022; 13(1): 4472.

[49]	Lin S, Bediako JK, Cho CW, Song MH, Zhao Y, Kim JA, et al. Selective adsorption of Pd(II) over interfering metal ions (Co(II), Ni(II), Pt(IV)) from acidic aqueous phase by metal-organic frameworks. Chem Eng J 2018;345:337-44.

[50]	Wei W, Reddy DHK, Bediako JK, Yun YS. Aliquat-336-impregnated alginate capsule as a green sorbent for selective recovery of gold from metal mixtures. Chem Eng J 2016;289:413-22.

[51]	Wei W, Cho CW, Kim S, Song MH, Bediako JK, Yun YS. PtIV, and Selective recovery of Au (III), Pd(II) from aqueous solutions by liquid-liquid extraction using ionic liquid aliquat-336. J Mol Liq 2016;216:18-24.

[52]	Lim CR, Lin S, Yun YS. Highly efficient and acid-resistant metal-organic frameworks of MIL-101(Cr)-NH₂ for Pd(II) and Pt(IV) recovery from acidic solutions: adsorption experiments, spectroscopic analyses, and theoretical computations. J Hazard Mater 2020;387:121689.

[53]	Lin S, Kumar Reddy DH, Bediako JK, Song MH, Wei W, Kim JA, et al. Effective adsorption of Pd(II), Pt(IV) and Au(III) by Zr(IV)-based metal-organic frameworks from strongly acidic solutions. J Mater Chem A Mater Energy Sustain 2017;5(26):13557-64.

[54]	Chen Y, Li Z, Ding R, Liu T, Zhao H, Zhang X. Construction of porphyrin and viologen-linked cationic porous organic polymer for efficient and selective gold recovery. J Hazard Mater 2022;426:128073.

[55]	Qiu J, Xu C, Xu X, Zhao Y, Zhao Y, Zhao Y, et al. Porous covalent organic framework based hydrogen-bond nanotrap for the precise recognition and separation of gold. Angew Chem Int Ed Engl 2023; 62(17): e202300459.

[56]	Liu L, Liu S, Zhang Q, Li C, Bao C, Liu X, et al. Adsorption of Au(III), Pd(II), and Pt (IV) from aqueous solution onto graphene oxide. J Chem Eng Data 2013; 58(2):209-16.

[57]	Zhang L, Zha X, Zhang G, Gu J, Zhang W, Huang Y, et al. Designing a reductive hybrid membrane to selectively capture noble metallic ions during oil/water emulsion separation with further function enhancement. J Mater Chem A Mater Energy Sustain 2018;6(22):10217-25.

[58]	Ding Y, Zhang S, Liu B, Zheng H, Chang C, Ekberg C. Recovery of precious metals from electronic waste and spent catalysts: a review. Resour Conserv Recycling 2019;141:284-98.

[59]	Niu B, Shanshan E, Xu Z, Guo J. How to efficient and high-value recycling of electronic components mounted on waste printed circuit boards: recent progress, challenge, and future perspectives. J Clean Prod 2023;415:137815.

[60]	Mann M, Nicholls TP, Patel HD, Lisboa LS, Pople JMM, Pham LN, et al. Sustainable gold extraction from ore and electronic waste. Nat Sustain 2025;8(8):947-56.

[61]	Zhou X, Cui Y, Xun X, Jia J, Wang XC, Quan ZJ. Selective recovery of precious metals through sulfur-rich ionic liquid polymers poly(S-[Vim-Br]). Separ Purif Tech 2025;365:132679.

[62]	Li Z, Zhao W, Li C, Yin Y, Wei D, Jin Y, et al. Electronegative strategic positions in covalent organic frameworks: unlocking high-efficiency gold recovery. Angew Chem Int Ed Engl 2025; 64(19):e202502199.

[63]	Majumder D, Fajal S, Shirolkar MM, Torris A, Banyla Y, Biswas K, et al. Nano-springe enriched hierarchical porous MOP/COF hybrid aerogel: efficient recovery of gold from electronic waste. Angew Chem Int Ed Engl 2025; 64(7):e202419830.

[64]	Liu M, Jiang D, Fu Y, Zheng Chen G, Bi S, Ding X, et al. Modulating skeletons of covalent organic framework for high-efficiency gold recovery. Angew Chem Int Ed Engl 2024; 63(1):e202317015.

[65]	Zalupski PR, McDowell R, Dutech G. The adsorption of gold, palladium, and platinum from acidic chloride solutions on mesoporous carbons. Solvent Extr Ion Exch 2014; 32(7):737-48.

[66]	Hong Y, Thirion D, Subramanian S, Yoo M, Choi H, Kim HY, et al. Precious metal recovery from electronic waste by a porous porphyrin polymer. Proc Natl Acad Sci USA 2020; 117(28):16174-80.

[67]	Zhang Z, Yang L, Li T, Meng Q, Wu Y, Zhou S, et al. Liquidambar formosana fruit-inspired hierarchical nano-trap framework for efficient uranium extraction from seawater. Matter 2025; 8(6):102055.