ABSTRACT The electrocatalytic CO 2 reduction reaction (CO 2 RR) to useful multicarbon (C 2+ ) products offers a way to help achieve carbon neutrality. Copper‐based catalysts are uniquely capable of achieving this efficiently; however, when used as single atoms or dual‐atom pairs, their structures change significantly during reactions. This change makes it difficult to apply traditional models that link a catalyst's shape to its performance, which hinders the design of high‐performance catalysts. To bridge this gap, this review presents a comprehensive framework focused on the behaviors and mechanisms of such dynamically evolving copper‐based catalysts in CO 2 RR. First, it explains how C 2+ products are formed at the atomic level, describing three main ways in which carbon atoms bond: symmetric, asymmetric, and single‐site dynamic coupling. Second, it summarizes the primary features that affect the degree to which these catalysts form C 2+ products, especially the changing environment and oxidation state (Cu + /Cu 0 ratio) during the reaction. Next, the discussion elucidates how external factors, such as electrolyte and electrolysis conditions, influence their dynamic surface reconstruction. Finally, emphasis is placed on the shift from passive observation to active catalyst design, driven by multiscale theoretical simulations and automated AI chemists. This offers practical insights into developing efficient atomically dispersed Cu‐based catalysts suitable for industrial use.
ABSTRACT Solar rechargeable flow batteries (SRFBs), which integrate solar energy conversion with electrochemical energy storage, have attracted increasing attention in recent years. To date, the reported photoelectrode‐based SRFBs predominantly employ either a single photoanode or a photoanode coupled with a silicon‐based photocathode for battery charging. Although silicon possesses an optimal bandgap and outstanding light‐harvesting capability, its intrinsic instability in aqueous environments and severe interfacial charge recombination necessitate complex and precisely engineered device architectures, thereby fundamentally limiting its scalability and practical deployment. Consequently, metal‐oxide photoelectrodes emerge as more viable candidates for SRFB applications. Herein, we report for the first time an SRFB architecture incorporating a Cu 2 O photocathode in conjunction with an iron‐oxide photoanode and the Fe(BPMG) 2 (II)/Fe(BPMG) 2 (III) and Fe 2+ /Fe 3+ redox couples. Benefiting from rational photoelectrode and interface design, the Cu 2 O photocathode delivers an applied‐bias photon‐to‐current efficiency (ABPE) of up to 0.48%. As a result, the assembled SRFB achieves an output voltage of 0.62 V and a solar‐to‐output electricity efficiency of approximately 0.11%. This work demonstrates the feasibility of employing metal‐oxide photocathodes in SRFB systems and provides a new design paradigm for the development of advanced photocathodes toward fully solar‐driven flow battery technologies.
ABSTRACT Electrochemical C−N coupling has emerged as a promising alternative to energy‐intensive synthetic routes for sustainable organonitrogen synthesis (e.g., urea, amides, amines, amino acids, oximes, and nitriles). By utilizing diverse carbon and nitrogen feedstocks, such as CO 2 and nitrogen oxides (NO x ), this approach advances carbon/nitrogen neutrality and simultaneously produces value‐added products. However, practical implementation remains challenging because of sluggish reactant adsorption, complex reaction networks, competing side reactions, and kinetic mismatches between carbon‐ and nitrogen‐containing intermediates. In this review, we validate rate matching as a critical design concept governing efficient C−N coupling and systematically summarize recent advances in the electrosynthesis of organonitrogen chemicals. We first review critical adsorbed intermediates and in‐depth C−N coupling pathways. Multidimensional engineering strategies are then categorized into catalyst‐, interface‐, and reactor‐level management and discussed, corresponding respectively to electrocatalyst design, electrolyte microenvironment modulation, and electrolyzer architecture. Furthermore, we elaborate on how the distinct functions of these strategies contribute to synchronizing C−N coupling. Finally, we conclude with remaining challenges and future perspectives toward efficient and scalable electrocatalytic synthesis of organonitrogen molecules.
ABSTRACT Real‐time monitoring of volatile molecular iodine (I2), a hazardous radioactive byproduct of nuclear processes, is critical for environmental and human safety. Fluorescence quenching offers a promising detection route, but conventional luminophores suffer from thermal instability at operational temperatures. Herein, we report a thermally robust zero‐dimensional antimony halide, [Sr2(18‐crown‐6‐ether)2(H2O)2(Cl2)]SbCl5, as the first luminescent sensor capable of real‐time I2 detection at elevated temperatures (348 K) in dynamic mode with a limit of detection (LoD) of ∼400 ppb, establishing a benchmark LoD value for high‐temperature iodine sensing via a luminescent technique. This material maintains structural integrity and intense [SbCl5]2− luminescence at 348 K, which is attributed to hydrogen‐bonding networks that suppress thermal quenching. In addition, the Sb(III) lone pairs serve as electron‐donating sites, capturing I2 to form polyiodides (i.e., I3− and I5−) via electron transfer, which triggers instantaneous luminescence quenching. This work establishes a new paradigm for high‐temperature optical sensors in nuclear safety applications.
ABSTRACT High‐energy‐density lithium metal batteries are of great interest as lithium‐ion batteries using graphite anodes are getting closer to their theoretical energy‐density limits. Poly(ethylene oxide) (PEO)‐based lithium metal batteries have the potential to achieve high energy density. However, their restricted electrochemically stable window, high operating temperature requirements, and low ionic conductivity in PEO limit their practical applicability. In this work, we combined polymer blending and organic‐inorganic composite modification to prepare a PEO/PVDF‐Al(OH) 3 composite quasi‐solid electrolyte. PVDF is uniformly dispersed within PEO, effectively reducing PEO crystallinity, while the lewis acidity of Al(OH) 3 promotes further dissociation of lithium salts. This enables PEO‐PNA3 to achieve an ionic conductivity of 2.72 × 10 −4 S cm −1 at 20°C. More importantly, the presence of [NMP‐Li + ] coordination mechanism in the electrolyte ensures favorable contact between the electrode and electrolyte interface, thereby promoting Li + transfer at the interface. At room temperature (approximately 25°C), the assembled Li/PEO‐PNA3/Li symmetric battery demonstrated stable cycling for 900 h at a current density of 0.2 mA cm −2 , whilst the LFP/PEO‐PNA3/Li battery cycled over 120 times at 0.2C current density. This work provides an effective and scalable strategy for designing high‐performance PEO‐based composite quasi‐solid electrolyte, offering valuable insights for developing high‐energy‐density lithium metal batteries.
ABSTRACT Industrial flue gases rarely contain only one type of toxic substance. Instead, alkali/alkaline‐earth metals, heavy metals, sulfur species, and phosphorus often coexist and interact with NH3‐SCR catalysts in a nonadditive manner. This review mainly summarizes the research progress on various poisons exposure over the past 5 years, with a focus on combinations involving anion and alkali/heavy metals, SO2 and alkali/heavy metals, alkali or alkaline‐earth metals and heavy metals, P and alkali/heavy metals, as well as combinations of heavy metals. Coexisting toxins often synergistically leads to catalyst deactivation. The main pathways include the concurrent loss of Brønsted and Lewis acidity of the catalyst, weakened redox ability, formation of chlorides or sulfates, pore blockage, and obstruction of electron and oxygen transport at the interface between the active phase and the support. Antagonistic effects also appear when toxic substances cross chelate into inert phases, such as Ca–As–O complexes or sulfates/phosphates of alkali/heavy metals. The active sites occupied by the toxic substances will be released and partially restore their adsorption and activation capabilities for reactants. From these cases, three practical strategies have emerged: establishing sacrificial capture domains for alkali and heavy metals, protecting the active phase with shells or layered porous carrier that intercepts deposit, and introducing co‐catalysts to enhance oxygen migration rate and acid‐site density, thereby maintaining the Langmuir–Hinshelwood and Eley–Rideal routes. These insights clarify the relationship between the structure and function of NH3‐SCR catalysts, and outline strategies for maintaining strong NH3‐SCR performance under typical mixed impurity conditions in sintering and other industrial flue gases.
ABSTRACT The photocatalytic conversion of methane (CH 4 ) into value‐added oxygenates without overoxidation under mild conditions remains a significant challenge in heterogeneous catalysis. Here, we rationally designed a series of S‐scheme MIL‐125‐NH 2 (Ti)/WO 3 ‐x (MW‐x) heterostructures via electrostatic self‐assembly for efficient CH 4 photooxidation. The direct S‐scheme charge transfer mechanism at the MIL‐125‐NH 2 (Ti)/WO 3 interface enhances spatial separation of photogenerated electron‐hole pairs, thereby optimizing redox efficiency. The WO 3 nanosheets, with their strong oxidative capacity, promote in situ H 2 O 2 generation from water, whereas the Ti 3+ /Ti 4+ redox centers in MIL‐125‐NH 2 (Ti) catalyze H 2 O 2 decomposition into hydroxyl radicals (·OH). These ·OH species efficiently activate the C–H bonds of adsorbed CH 4 , yielding methyl radicals (·CH 3 ). The concurrent generation and coupling of ·OH and ·CH 3 radicals drive selective formation of C 1 oxygenates. Notably, the optimized MW‐3 catalyst exhibits exceptional performance, achieving a total C 1 oxygenate yield of 502.17 μmol·g cat −1 under ambient conditions, surpassing most reported photocatalysts for CH 4 conversion.
ABSTRACT Thermochromic materials are gaining increasing interest with the merits of adaptive optical response to temperature/heat, with potential applications in thermal indicators, energy‐efficient smart windows, thermal distribution monitors, laser warning markers, etc. Transition metal compounds are the most classic inorganic pigments known since prehistoric culture. In this review, we summarize the recent research progress of inorganic thermochromic materials, especially focused on transition metal compounds. The performance of inorganic thermochromic materials is closely related to their crystal structure and electronic structure, especially the d‐orbital electrons of transition metals, which play a key role in the response to temperature changes. The classification based on the composition, mechanism, and working principles of the thermochromic materials is clarified first. Then, the materials based on different transition metal compounds are summarized for varied d‐electron configurations of transition metal cations in binary and multinary metal oxides, halides, sulfides, and salts. The mechanisms of thermochromism are summarized accordingly, including phase transition, charge transfer, and bandgap change. Then, the applications in the fields such as smart windows, radiative cooling, and temperature sensing are reviewed. Finally, we propose a perspective on the challenges and future development directions in the design, fabrication, and applications of thermochromic materials.
ABSTRACT The escalating concentration of atmospheric CO 2 has intensified the search for solar‐driven routes that convert carbon dioxide into value‐added fuels and chemicals. Photocatalytic CO 2 reduction offers a direct pathway toward carbon circularity; however, its realization is fundamentally constrained by inefficient charge separation, multielectron transfer requirements, competitive hydrogen evolution, and limited control over reaction selectivity. Polyoxometalates (POMs) have emerged as uniquely versatile platforms in this context due to their structurally programmable metal‐oxo frameworks and reversible multielectron redox chemistry. Acting as molecular electron reservoirs, charge‐transfer mediators, and coordination‐defined catalytic microenvironments, POMs provide an unusually direct handle over proton‐coupled electron transfer processes central to CO 2 activation and reduction. This review critically examines the roles of POMs across molecular, hybrid, and composite photocatalytic architectures. We categorize POM‐enabled systems into (i) intrinsic POM photocatalysts, (ii) photosensitizer‐assisted assemblies where POMs function as redox relays and electron buffers, (iii) POM‐metal‐organic complexes, and (iv) POM‐integrated semiconductor and MOF/COF heterostructures. By correlating structural motifs with charge‐regulation behavior, interfacial electron transport, and product distribution, we elucidate how POMs reshape reaction pathways and selectivity landscapes. Finally, we identify emerging design principles and outstanding challenges for advancing POM‐centered photocatalysts toward efficient visible‐light‐driven CO 2 conversion.
ABSTRACT A bimetallic NiAg alloy is assembled on the surface of Zn3In2S6 to construct a NiAg‐Zn3In2S6 composite using a chemical reduction method. By adjusting the different alloy ratios, the hydrogen evolution activity of the optimum Ni0.25Ag0.75‐Zn3In2S6 photocatalyst achieves 21.32 mmol·g−1·h−1, which is 12.5, 3.8, and 1.7 times higher than those of pure Zn3In2S6 (1.7 mmol·g−1·h−1), Ni‐Zn3In2S6 (5.5 mmol·g−1·h−1), and Ag‐Zn3In2S6 (12.3 mmol·g−1·h−1), respectively. The apparent quantum efficiency (AQE) of the optimum Ni0.25Ag0.75‐Zn3In2S6 photocatalyst is 15.1% and 6.8% under monochromatic light at wavelengths of 370 and 456 nm. Systematic experiments and DFT theoretical calculations demonstrate that the plasmon hybridization of the loaded NiAg alloy can significantly improve the light‐trapping ability of Zn3In2S6. The introduction of NiAg alloy optimizes the carrier transport paths, acts as a trapping site for the photoinduced electrons, and reduces carrier recombination, thus enhancing the photocatalytic performance of the catalysts. Furthermore, the NiAg alloy improves H adsorption on both Ni and Ag and provides more optimal Ag sites as active sites for H adsorption. This approach demonstrates the feasibility of replacing precious metals with cost‐effective, earth‐abundant NiAg alloys as efficient cocatalysts for modifying Zn3In2S6, holding promising potential for photocatalytic hydrogen evolution applications.
ABSTRACT At present, the low temperature reactivity and resistance to SO 2 poisoning performance of environmentally friendly Ce‐based catalysts in the NH 3 ‐SCR reaction are still the main factor for practical application. In this work, Fe 3+ was introduced into the TiO 2 lattice using the hydrothermal method and substituted for part of Ti 4+ to form oxygen‐deficient structure in the Fe‐TiO 2 carrier, and active species CeW were loaded onto this defective carrier to test its catalytic performance. It was demonstrated that CeW/Fe‐TiO 2 catalyst with higher oxygen vacancy content exhibited better low temperature catalytic activity and superior resistance to SO 2 poisoning in NH 3 ‐SCR reaction. On the one hand, O v was able to optimize the electronic structure of the catalyst with electron enrichment in the Fe‐O v ‐Ti structural unit and electron transfer to surface Ce atom through oxygen vacancies, thus improving the chemical environment around Ce species. On the other hand, O v effectively adsorbed and activated oxygen and reactant molecule, and the NH 3 ‐SCR reaction proceeded through L‐H pathway, thus improving the low temperature performance of the CeW/Fe‐TiO 2 catalyst. Eventually, DFT results confirmed at the molecular level that the construction of oxygen vacancy defective structures effectively activated the reactant molecules and thus improved the catalyst efficiency.
ABSTRACT Electrochemical reduction of CO 2 into value‐added chemicals using renewable electricity offers a promising pathway for sustainable fuel production, yet its industrial implementation has been hindered by lack of efficient and stable catalysts. Here we present a series of silver nanoparticles (Ag NPs) modified 2D conductive Cu‐MOF, namely Cu 3 (HHTP) 2 (H 6 HHTP = 2,3,6,7,10,11‐hexahydroxytriphenylene), demonstrating enhanced catalytic activity and selectivity. The optimized Ag@Cu 3 (HHTP) 2 composite exhibits superior electrocatalytic performance, achieving a Faradaic efficiency (FE) of 65.1% for CH 4 production at commercially relevant current density (−240 mA cm −2 ) while maintaining stable operation for 24 h under industrial‐grade current density. Mechanistic investigations show that the incorporation of Ag NPs induces dual‐functional effects: (1) electronic structure optimization through interfacial charge redistribution and (2) enhanced CO 2 adsorption and activation capacity. This study establishes a fundamental paradigm for designing high‐performance MOF‐based electrocatalysts for CO 2 reduction through rational metal decoration strategy.
ABSTRACT Cocatalyst structure is crucial for optimizing the utilization of photogenerated charge carriers to enhance photocatalytic efficiency. Here, we reported an amorphous flower‐like hollow structure cocatalyst CoZnP x ‐H with a large capacitance of 8.5 F/g about 19.7 times of that solid crystalline CoZnP x . The photocatalytic H 2 production rate of CoZnP x ‐H loaded on CdS achieves 54.0 mmol/g/h, which is 4 times greater than that of CoZnP x loaded on CdS. Interestingly, during the photocatalytic production, the simultaneous acetic acid rate from CoZnP x ‐H/CdS arrives at 64.1 mmol/g/h, which is 2.2 times greater than that from CoZnP x /CdS. The excellent cocatalytic performance of CoZnP x ‐H can be contributed to the strong capacitance, large surface area, excellent hydrophily brought about by its specific structure. The strong capacitance is beneficial for storing photo‐excited electrons, thus facilitating the efficient separation of photogenerated charges. The large surface area and excellent hydrophily provide abundant reactive sites and easy contact with reactants for proton reduction. As a result, the capacitance catalysis effect and surface redox kinetics improve, and the hydrogen and acetic acid simultaneously generate. This study proposes an effective strategy of modulating the cocatalyst structure to simultaneously obtain H 2 and high‐value‐added chemicals.
ABSTRACT Water‐mediated photothermal CO 2 reduction to CH 4 is promising for renewable energy storage and carbon neutrality, but its selectivity and efficiency are limited by sluggish water dissociation that serves as a critical proton source and the demanding eight‐electron transfer barrier of CH 4 formation. These issues lead to insufficient protons for *CO hydrogenation. Herein, we engineer subnanoscale CeO 2 ‐Cu 2 O heterostructured subnanowires with densely enriched CeO 2 ‐Cu 2 O interfaces to overcome this proton bottleneck. Experimental and theoretical simulation results demonstrate that these interfaces accelerate H 2 O dissociation and create a “proton‐rich microenvironment,” which boosts the proton supply rate to match the kinetic demand of *CO hydrogenation. This directs the protonation of *CO to *CHO instead of CO desorption; these intermediates then convert to *CH 2 O and *CH 3 O, achieving over 99% CH 4 selectivity and a record yield of 2818 μmol g −1 h −1 . This yield is 15‐fold higher than that of bulk and nanoparticle counterparts, underscoring the key role of subnanoscale interface enrichment in optimizing multielectron reactions.
ABSTRACT With the rapid development of photovoltaic (PV) technologies, the storage and transportation of the electricity generated by photovoltaics have received increasing attention. Advanced technologies that integrate photovoltaic energy conversion and storage are important for handling the regional and intermittent features of solar energy, thereby enabling its efficient utilization. Recently, photovoltaic‐driven electrocatalytic water splitting (PV–EC) for hydrogen production has been considered one of the most promising technologies. A deep understanding of both photovoltaic systems and electrocatalytic water splitting systems is essential for designing and evaluating a highly efficient photovoltaic‐driven electrocatalysis (PV–EC) system. This review aims to provide key knowledge and guidance on PV–EC systems. It begins by introducing the characteristics of various photovoltaic technologies, which would offer guidance on selecting the most suitable PV system for matching with the electrolysis process. It then analyzes the principles, advantages, and drawbacks of various PV–EC configurations, along with strategies for effectively coupling PV and EC units. This would provide guidance on regulating operating conditions in PV–EC systems. Finally, it discusses the challenges that hinders high solar‐to‐hydrogen efficiency and suggests future research directions to enhance practical applications.
ABSTRACT Ultra‐deep heavy oil is an important unconventional resource, but its extremely high viscosity, poor mobility, and the high energy demand for conventional recovery methods severely limit its efficient and sustainable production. To address these limitations, a triflate‐functionalized Ni–Ce/MOF superacid catalyst (Ni–Ce/MOF–OTf), based on a UiO‐66(Ce)–type (BTC‐based) framework, was developed to enable low‐temperature in situ upgrading under near‐reservoir conditions. The catalyst was synthesized through a two‐step post‐synthetic modification route using a Ni–Ce/MOF precursor, involving acid activation followed by grafting of triflate groups onto the framework. This design was intended to integrate strong Brønsted acidity, tunable Ni/Ce Lewis acid sites, and pore confinement within a single catalytic microenvironment, thereby promoting selective bond cleavage and suppressing secondary repolymerization. Under reservoir‐mimicking conditions (∼140°C), Ni–Ce/MOF–OTf achieved a viscosity reduction of 92.11% within 12 h, maintained viscosity rebound below 10% over 60 days, and retained about 80% of its activity after four cycles. Structural characterization and theoretical calculations showed that triflate functionalization enhanced acidity, increased oxygen vacancy density, and strengthened metal–ligand interactions, enabling efficient cleavage of C–C/‐C–C, C–S, and C–O bonds at a lower temperature. Core‐scale physical simulation further demonstrated a recovery factor of 90.25% through gas‐assisted catalytic upgrading. In addition, techno‐economic and cradle‐to‐wellhead assessments indicated improved economic competitiveness and the lowest cradle‐to‐wellhead carbon footprint among the evaluated heavy oil recovery routes. These results demonstrate an effective materials–reaction–engineering strategy for cleaner and more sustainable utilization of ultra‐deep heavy oil.
ABSTRACT Efficient conversion of carbon dioxide to organics has been a promising outlet for value‐added carbon dioxide consumption. However, most of the catalysts developed for this process currently focus on expensive noble metal catalysts, which severely limits their further evolution and application. Herein, a precisely designed dual‐stabilized single‐site Fe(II) catalytic system is developed through combination of the covalent interaction between the β‐diketiminate ligand and the hyperactive Fe(II) center and the host–guest interaction between the porous matrix and active species, which realized the most efficient production of propiolic acid from CO2 and terminal alkynes under ambient conditions with stable multiple recycling. The advantages of both homogeneous and heterogeneous catalysts are achieved in a single‐site Fe(II) catalytic system, whose performance surpasses the known noble metal catalysts in terms of yield. Density functional theory model calculations are employed to explore the optimal pathways and mechanisms for the catalytic conversion of CO2 to propiolic acid over the prepared catalytic platform.
ABSTRACT Developing efficient, low‐cost electrocatalysts for overall water splitting (OWS) is critical for advancing hydrogen energy technologies. Here, we fabricate Mo‐incorporated N‐rich‐CoMoCN electrocatalyst from ZIF‐67 (CoCN material), ammonium molybdate, and melamine precursors. This catalyst, featuring the predominant Co/Co 6 Mo 6 C 2 heterojunction and abundant surface‐layered architecture, collectively provides an ideal microenvironment for catalytic reactions and facilitates charge transfer. In alkaline media, it exhibits outstanding bifunctional activity, delivering overpotentials of only 107 and 256 mV for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, at a current density of 10 mA cm −2 , far surpassing the performance of CoCN and CoMoCN. Notably, the N‐rich‐CoMoCN‐based electrolyzer requires only 1.52 V to achieve 10 mA cm −2 in a two‐electrode system with 1.0 M KOH. The comprehensive structural and electrochemical characterizations reveal that the incorporation of Mo and N modulates the catalyst's morphology as well as lattice and electronic configurations, resulting in the strong electronic interaction between Co, Mo, and N, thereby accelerating the intrinsic reaction kinetics. Density functional theory (DFT) calculation further uncovers that N enrichment can effectively modulate the electronic state distribution of Co and Mo, thereby promoting interfacial charge rearrangement and regulating the d ‐band center of the catalyst. The synergistic effect between heterostructure construction and N enrichment optimizes the electronic structure and surface energy of the N‐rich‐CoMoCN catalyst, which facilitates charge transfer, ultimately leading to enhanced electrocatalytic activity in OWS performance. This work highlights an efficient strategy for designing high‐performance bifunctional catalysts from MOF‐derived heterostructures for sustainable hydrogen production.
ABSTRACT The pursuit of ultra‐high energy‐dense lithium‐metal batteries (LMBs) has reignited the drive to fabricate ultrathin high‐quality lithium metal anodes. This review critically evaluates four representative manufacturing techniques: extrusion, molten lithium infusion, electroplating, and physical vapor deposition (PVD). We analyze each method across key performance metrics—thickness control, purity, interfacial uniformity, scalability, and cost efficiency—to highlight their unique trade‐offs. Extrusion offers robust scalable foils with mechanical homogenization, whereas molten infusion enables conformal penetration into 3D porous hosts. Electroplating delivers exceptional control over nucleation and morphology via electrolyte engineering and interfacial design. PVD methods (thermal evaporation, sputtering, and pulsed‐laser deposition) afford atomically clean films with precise microstructural tuning. Despite substantial advances in each route, significant challenges remain—including large‐area manufacturing, long‐term solid‐electrolyte interphase stability, and cost‐effective scaling. We propose a forward‐looking roadmap centered on hybrid manufacturing strategies, operando and in situ diagnostics, sustainability assessment, and safety and regulatory frameworks. By synergizing the complementary advantages of different approaches, we argue that a holistic manufacturing paradigm can accelerate the translation of lithium metal anodes from laboratory‐scale demonstrations to industrially viable high‐energy battery systems.
ABSTRACT The rapid consumption of electronic products has led to a significant accumulation of electronic waste (e‐waste) that contains a considerable amount of gold (Au). Recovery of Au from e‐waste is significant for the potential sustainability of industry and society. Porous organic polymers (POPs) recently show promising applications in Au recovery; most of them are designed as neutral structures. Here, we report an ion‐enriched POP (PiP‐1) through the polycondensation of the ionic guanidine‐based and imidazole‐based building blocks. Attributed to its highly charged frameworks, PiP‐1 displays ultrahigh Au adsorption capacity of 1530.9 mg g−1, with excellent selectivity and recyclability. Moreover, PiP‐1 also shows promising selective capture ability toward Au3+ ions in the actual CPU leaching solution test. Our work illustrates that developing high ion‐density frameworks could be an efficient strategy to enhance the Au adsorption performance, and ionic POPs hold great potentials as gold adsorbents from actual e‐waste.
