ABSTRACT Bio‐based adhesives are gaining traction by virtue of their tremendous potential for substituting petrochemical adhesives, yet the restricted adhesion performance, poor water retention, and intrinsic flammability severely hindered their scale‐up application. Herein, drew inspiration from gecko setae and biomineralization, a novel bio‐based adhesive derived from epoxidized HEC‐core hyperbranched polyester hybrid (EH), gelatin (G) and modified nano‐hydroxyapatite (γHA) is presented. In this system, the self‐synthesized EH features a setae‐like hyperbranched structure enriched with abundant active groups, which maximize interfacial effectiveness. Meanwhile the gelatin and hydroxyapatite act synergistically achieve marked enhancements in robust cohesion and durable water retention via biomineralization. The developed organic‐inorganic hybrid adhesive offers a unique combination of broad substrate universality, low‐temperature curability, satisfactory flame retardancy, outstanding environmental robustness, and superior storage stability. The integrated performance profile enables wide‐temperature on‐demand bonding, safe construction application, and extended practical utility with reliable long‐term performance. This bioinspired strategy represents a fresh and feasible insight for the promotion of bio‐based adhesive, and offers a prospective pathway toward robust, sustainable, and safety versatile bonding materials.
Deep eutectic solvent (DES)-derived quaternized cellulose nanofibers (QCNFs) were used to electrostatically assemble carboxylated multiwalled carbon nanotubes (MWCNTs) to fabricate polyacrylamide (PAM)-based conductive hydrogels for strain sensing. The hybrid network lowers the percolation threshold, resulting in a conductivity of 2.75 mS cm-1, a toughness of 431 kJ m-3, a response time of 200 ms, and a gauge factor of up to 6.64 for wearable motion monitoring.
Eutectogels hold considerable promise soft electrodes for high-performance flexible triboelectric nanogenerator (TENG) due to their tunable mechanical properties and environmental stability. However, conventional eutectogels with single linear polymer chains often exhibit poor mechanical strength as well as undesirable migration of components (e.g., initiators), which compromise device stability and limit their environmental adaptability in high-performance energy harvesting. Here, lignin was molecularly engineered into branched lignin nanospheres (BLNS) functionalized with polymerizable acrylate groups. In a deep eutectic solvent system, BLNS simultaneously enabled rapid self-initiated UV polymerization (97.3% C--C conversion) and constructed a robust, nonmigrating crosslinked network, yielding triboelectric supramolecular eutectogels (SEG). Specifically, benefiting from branched backbone and nanoreinforcing effect of the BLNS, the resulting SEG achieved exceptional mechanical robustness (tensile strength of 1.76 MPa, toughness of 5.10 MJ/m3) and strong adhesion (1.21 MPa). The SEG-based sensor exhibited a high ionic conductivity of 4.50 mS m- 1 and a gauge factor of 3.3, while maintaining stable sensing performance over a wide temperature range (-30 to 80 degrees C) and under varying humidity conditions (30-90% RH), demonstrating excellent adaptability to harsh environmental conditions. As a proof-of-concept, a TENG was constructed using the SEG as the flexible electrode, with open-circuit voltage remaining stable over 6000 contact-separation cycles, underscoring the robustness and operational stability essential for reliable self-powered soft electronic systems. This work establishes a versatile strategy for designing multifunctional lignin-based materials for next-generation self-powered electronics.
Aqueous zinc ion batteries (AZIBs) utilizing hydrogel electrolytes have emerged as promising sustainable solutions for flexible energy storages owing to their intrinsic safety and mechanical stability. However, the inherent poor toughness, low Zn2+ transference number, and lacking electron field regulation capability in conventional hydrogel electrolytes exacerbate uncontrolled Zn dendrite growth and side reactions, posing a substantial challenge to interfacial stability between the Zn anode and the hydrogel electrolyte. To address this, here we present a novel biphasic hydrogel electrolyte capable of both multi-scale stress deconcentration and dual-field regulation via polymerization followed by salting-out and coordination strategy. The well-designed hydrogel electrolyte demonstrates high toughness of 17.5 kJ m(-2), an ionic conductivity of 60.6 mS cm(-1) and a Zn2+ transference number of 0.753, collectively achieving highly reversible Zn plating/stripping and exceptional interfacial stability. Consequently, the Zn||NaV3O8 center dot 1.5H(2)O (NVO) full cells equipped with this hydrogel electrolyte show remarkable electrochemical performance, including high capacity (375.4 mAh g(-1) at 0.5 A g(-1)), outstanding rate capability (188.9 mAh g(-1) at 8 A g(-1)) and long-term cycling stability (91.6 % capacity retention after 3000 cycles), with sustained performance under harsh conditions such as high temperature, high humidity, and low temperatures (-30 degrees C). Furthermore, the assembled flexible pouch cells demonstrate exceptional mechanical and environmental adaptability, reliably powering a circular lamp even under severe bending at both room and -30 degrees C. This work provides fundamental insights into Zn anodic chemistry in multifunctional hydrogel electrolyte and offers practical guidelines for constructing advanced zinc-based energy storage devices.
The practical application of wood-based materials in sustainable triboelectric nanogenerators (TENGs) is constrained by their mechanical weakness, poor environmental tolerance, and insufficient electrical output. Incorporating functional polymers offers potential for enhancing wood-based substrates, yet weak interfacial bonding often undermines structural stability. Herein, we develop an optimized wood-based substrate (WS) featuring superior mechanical toughness, water resistance, and transparency by constructing the biomimetic hierarchical structures. The filler matrix, engineered with reactive isocyanate groups, enables the formation of stable covalent bonds at hierarchical interfaces, thereby achieving exceptional mechanical toughness (3.38 MJ/m3), water resistance, and a high dielectric constant (5.33). Leveraging these properties, the WS serves as a sustainable substrate for a rotary TENG, enabling efficient wind and water flow energy harvesting, and achieving a significantly enhanced peak power density (300.7 mW/m2) compared with most of the reported wood-based TENGs. This work opens up new avenues for designing next-generation wood-based TENGs for efficient green energy harvesting.
Abstract Lignin-containing cellulose nanofibers (LCNFs) offer a sustainable alternative to fully delignified nanocellulose by preserving native lignin while reducing chemical and energy consumption. Herein, bamboo-derived LCNFs were prepared through a one-step maleic anhydride esterification without toxic solvents or catalysts. The resulting LCNFs exhibit high lignin content (27.14%), abundant surface carboxyl groups (1.85 mmol g−1), ultrafine diameters (∼2.67 nm), and high aspect ratios (>1 μm), enabling excellent dispersion and strong interfacial interactions with polymer networks. When incorporated into poly(acrylamide-co-lauryl methacrylate) hydrogels, the LCNFs function as dual-functional crosslinkers by simultaneously providing covalent anchoring sites and physical entanglement points. The synergistic interactions significantly enhance the mechanical robustness and electrical performance of the hydrogels, yielding a tensile strength of 1.12 MPa, elongation at break of 1545%, toughness of 7.33 MJ·m−3, and electrical conductivity of 1.15 S/m. Multiscale analyses reveal that the reinforcement originates from cooperative hydrogen bonding, covalent coupling, and nanoscale network interpenetration induced by LCNFs. This work demonstrates a green and efficient strategy for converting bamboo biomass into functional LCNFs and highlights their potential as sustainable reinforcing and crosslinking components in high-performance conductive hydrogels for flexible sensing and wearable applications.
The use of non-degradable polymer films has raised urgent environmental concerns, prompting the development of biodegradable alternatives with robust mechanical performance; however, the heterogeneous structure and poor interfacial compatibility of lignin often limit its reinforcing efficiency in polymer matrices. Herein, a green γ-valerolactone-gallic acid solvent system was developed for in situ lignin modification during pretreatment, enabling controlled structural reorganization and interfacial engineering within the polyvinyl alcohol (PVA) matrix. GA incorporation increased the density of polar functional groups and enhanced hydrogen bonding interactions with PVA chains, leading to improved interfacial compatibility and a more uniform polymer network. The resulting film demonstrated improved mechanical properties-tensile strength (∼46 MPa), Young's modulus (0.22 GPa), and toughness (70 MJ·m-3). Lignin integration enhanced water resistance and imparted efficient photothermal conversion, enabling stable cyclic heating under solar irradiation. This strategy provides a viable approach for developing biodegradable films that combine mechanical integrity with multifunctionality.
To alleviate the dependence of commercial adhesives (e.g., phenol-formaldehyde and urea-formaldehyde resins) on fossil resources, substantial research efforts have focused on developing lignin-phenol-formaldehyde (LPF) resins. Owing to the low reactivity of condensed technical lignins (e.g., kraft and organosolv lignins), LPF resins continue to suffer from structural heterogeneity, inferior bonding performance, limited phenol substitution rate, and formaldehyde emissions. Given that lignin functions as a natural binder to endow higher plants with structural rigidity and water resistance, extracting native-like lignin from lignocellulosic biomass therefore offers a promising route towards fully bio-based alternatives. However, simultaneously achieving green lignin extraction and practical bonding performance of the resulting adhesives remains elusive. Here we report an effective strategy to overcome this trade-off. Our approach involves protecting lignin with L-cysteine in an aqueous formic acid system during biomass fractionation, followed by simply dispersing the resulting L-cysteine-protected lignin (CPL) in water. Among fossil-free all-lignin adhesives, the resulting CPL adhesive achieves a record wet bonding strength of 1.48 MPa and an exceptional dry bonding strength of 1.85 MPa. Multi-layer plywoods that bonded with this adhesive also exhibit superior flexural resistance, long-term stability, and negligible formaldehyde emissions. Mechanistically, L-cysteine forms C–S bonds at the α-positions of lignin during fractionation, which controls the initial molecular weight of CPL via inhibiting condensation reactions, and preserves its active linkages (e.g., aryl ether bonds) and functional groups (e.g., hydroxyl and carboxyl groups). These structural features facilitate the penetration, in situ depolymerization and condensation of lignin, as well as non-covalent interactions during hot pressing, thereby enabling the high-performance adhesion of CPL adhesive towards wood veneers.
Lightweight, high-strength composites with plant fibers as the reinforcing phase still generally have the problems of non-biodegradable matrix and poor compatibility at the interface between fibers and polymers. In this study, a moldable biodegradable and high-strength all-bamboo fiber composites (ABFCs) was fabricated using bamboo fibers as the reinforcing phase and sodium periodate-activated bamboo fibers (AF) as the matrix phase through an aqueous-phase mixing and hydrothermal molding process. ABFCs exhibit excellent mechanical properties, including a tensile strength of 110.60 MPa, flexural strength of 157.95 MPa, flexural modulus of 15.11 GPa, impact strength of 12.34 kJ/m2, and Shore hardness of 95 HD. ABFCs exhibit strength more than twice that of traditional bamboo-plastic composites, due to strong interfacial bonding between bamboo fibers and the AF matrix, which enables effective load transfer and dispersion. It also shows excellent solvent resistance, maintaining shape stability after 45 days of immersion. Meanwhile, ABFCs can biodegrade in soil within 120 days and chemically degrade rapidly within 12 h in a 1 % NaOH. Moreover, ABFCs can be recycled through crushing and re-molding via hydrothermal hot pressing. This work offers a sustainable solution that enhances the utility of bamboo while addressing plastic pollution.
Natural plant cells featuring polygonal honeycomb architectures exhibit exceptional load-bearing and energy dissipation capacities. The strategic incorporation of this biomimetic structure presents an effective reinforcement approach for composite materials. In this study, a fully biobased and sustainable soy protein adhesive with improved water resistance and bonding strength was developed through the integration of modified cork. The cork was modified via a two-step process: deep eutectic solvent treatment to partially remove lignin while preserving the unique cellular framework, followed by dopamine hydrochloride functionalization to improve interfacial reactivity and promote extensive hydrogen bonding with the soy protein matrix. The resulting composite adhesive demonstrated remarkable improvements in performance, achieving a wet shear strength of 1.15 MPa and a 111.8% increase in fracture toughness compared with unmodified soy protein adhesive. This work provides an effective strategy for fabricating high-performance, fully biobased adhesives and highlights the value-added utilization of cork as a functional reinforcement material.
Bamboo cellulose exhibits excellent biocompatibility and renewability, making it a promising alternative to conventional non-renewable petroleum-based resources. However, the inherent trade-off between strength and toughness, together with the flammability of cellulose, poses significant challenges for the development of bamboo cellulose-based films that simultaneously exhibit high strength, high toughness, and flame retardancy. In this study, a multiscale strategy involving deep eutectic solvent treatment is employed to deconstruct, modify, and reconstruct the bamboo cellulose network, thereby transforming it into a high-performance bioplastic. First, phosphorylated cellulose fibers with different size scales were prepared using a reactive ternary deep eutectic solvent. Subsequently, a film was successfully constructed via a micro/nano scale design strategy involving the physical entanglement of cellulose microfibrils and the physical filling of cellulose nanocrystals. The resulting film exhibits high strength (82.32 MPa), high toughness (20.05 MJ m-3), excellent flame retardancy (LOI = 62.17%), as well as outstanding thermal stability, biodegradability, and recyclability, outperforming most reported cellulose-based flame-retardant films. This study demonstrates the significant promise of bamboo biomass as a sustainable substitute for petroleum-derived materials, thereby advancing the transition toward high-value applications of bamboo cellulose.
Lignin-based carbon nanospheres have been considered as ideal electrode materials for supercapacitors because of regular morphology and high specific surface area. Heteroatom-induced defects on the carbon chain can resolve the poor hydrophilicity and surface functional group deficiency of pure carbon nanospheres, improving electrochemical performance. Herein, nitrogen and phosphorus co-doped lignin-based carbon nanospheres (NPCS) with different doping content were constructed by solvent exchange, hydrothermal treatment and carbonization treatment. The results showed that the NPCS could maintained perfect spherical morphology and good dispersion. When the ratio of covalent-bond stabilized lignin nanospheres to ammonium dihydrogen phosphate was 1:1 and the carbonization temperature was 700 degrees C, the optimal specific surface area (89.8 m2 g- 1) and doping ratio of nitrogen and phosphorus (14 at%) were demonstrated in the NPCS. The obtained NPCS showed excellent capacitance storage capacity (312 F/g at 0.2 A/g) and significant cycle stability (93.7% capacitance retention after 10,000 cycles). The symmetric capacitor assembled based on NPCS had an energy density of 4.9 Wh /kg at the power density of 129.8 W/kg. This is mainly attributed to the fact that the NPCS has a high specific surface area and an enhanced affinity toward K ions. The study presents a novel approach to heteroatom co-doping in lignin-based carbon nanospheres, highlighting their potential for use in electrode materials.
Gel electrolytes are high-priority materials for solid-state Zn-ion hybrid capacitors, characterized by high ionic conductivity and intrinsic mechanical flexibility. However, because the existing gel electrolytes are relatively soft and do not contact intimately with rigid Zn anodes, they have inferior interfacial compatibility with Zn anodes, leading to device degradation. Here we develop a class of biogel electrolytes by in situ crystallizing gelatin triple helix units from the alginate polymer domain to form a unique hierarchical-heterogeneous structure. The biogel electrolyte demonstrates combined advantages of high toughness, temperature-triggered adhesion, high Zn2+ transference number and temperature-independent ionic conductivity. These notable features favor Zn2+ 3D diffusion and accommodate zinc anode volume changes, thus enabling the symmetric Zn||Zn cell to highlight a balance among high current density, high areal capacity and prolonged cycling life. Moreover, the assembled zinc||activated carbon hybrid capacitor performs exceptional capacitive behavior and stable operation across the temperature range from 25°C to -40°C, delivering competitive energy density of 125.5 Wh kg-1 with high capacity retention of 97.1% over 10 000 cycles even at -40°C. Finally, system-level demonstration based on the resulting hybrid capacitors can power portable electronics in a power cable-free manner, validating applicability for green power sources in outdoor activities.
Constructing a water-in-oil (W/O) emulsion adhesive offers a promising strategy to mitigate bondline starvation and interfacial discontinuity resulting from excessive isocyanate penetration into wood in laminated systems. However, the reactive isocyanate-water heterogeneous interface leads to premature NCO consumption, uneven network formation, and interfacial defects. Therefore, reconciling adhesive retention with controlled interfacial reactivity remains a key challenge. Here, inspired by the structural logic of cell membranes in compartmentalizing phases and organizing interfaces, we design lignin colloids as multifunctional regulators in emulsions and establish a cooperative strategy that couples bulk rheological regulation with interfacial film engineering. Owing to their amphiphilic surface chemistry and steric effects, lignin colloids increase the apparent viscosity of the continuous isocyanate phase to suppress overpenetration while enriching at the isocyanate-water interface to assemble into an interfacial film. This film spatially limits direct phase contact and temporally buffers interfacial reactions. Consequently, the penetration depth in wood decreased from around 200 to 25 μm, the pot life of the emulsion was extended by 1.5-2-fold compared with the additive-free system, and about 80% of NCO was retained. A clear and continuous bondline structure was formed after curing, with dry shear strength increasing from 1.02 to 1.74 MPa. The strength retention rate after boiling water treatment reached 93%, and the system demonstrated greater environmental durability. Notably, the isocyanate usage can still be reduced by 30% while delivering enhanced bonding performance, highlighting the potential of this strategy for efficient wood adhesive systems with reduced isocyanate input.
Soybean meal (SM) adhesives are regarded as promising alternatives to petroleum-based adhesives for promoting the sustainable development of the wood industry. However, the conflict between the high cross-linking efficiency of cross-linkers and the pot life of adhesives severely limits the industrial application of SM adhesives. Herein, a pressure-triggered microcapsule cross-linking strategy was proposed. Pressure-responsive PAPI microcapsules with reactive cores were prepared through interfacial polymerization between chain extenders and polymeric methylene diphenyl diisocyanate (PAPI), and subsequently incorporated into SM adhesives to construct a pressure-triggered cross-linking system. The mechanism underlying stable encapsulation and pressure-triggered release was clarified by analyzing the interfacial chain-extension reaction, shell characteristics, core retention, and pressure-induced morphological changes of the microcapsules. The microcapsules prepared using polyethylene glycol 200 as the chain extender and an emulsification speed of 1400 rpm exhibited suitable shell stability and effective pressure-triggered release behavior. Moreover, tannic acid (TA) was introduced to enhance the mold resistance and further improve the bonding performance of the adhesives through TA-induced non-covalent interactions. The developed adhesive still maintained a wet shear strength of 0.74 MPa after 24 h of storage. Meanwhile, the pot life of the adhesive was prolonged by 12 times compared with that of conventional cross-linking SM adhesives. This work provides a new strategy for developing sustainable protein-based adhesives with both high bonding strength and long pot life, reducing resource waste and improving production continuity.
Triboelectric nanogenerators (TENGs) from bioderived polymers offer a sustainable route for energy harvesting. Specifically, vegetable oil-based polymers (VOPs) combine renewability with flexibility, yet their high viscosity and poor mechanical strength have impeded the fabrication of robust, high-surface-area architectures essential for efficient devices. To overcome this, we designed a hyperbranched one-component nanocomposite (HOCN) by covalently grafting VOP chains onto cellulose nanofibrils (CNFs). By enabling the stable electrospinning of high-oil-content VOPs, the HOCN architecture concurrently addresses key processing challenges: reducing viscosity, enhancing conductivity, and reinforcing the network. Consequently, the resulting membranes exhibit a tensile strength of 0.6 +/- 0.1 MPa and a toughness of 2.6 +/- 0.3 MJ/m3, a nearly 6-fold improvement over pure PLT membranes. Integrating carbon nanotubes (CNTs) into this network produces a flexible, self-supporting triboelectric layer that couples efficient charge induction with rapid electron transport. The optimized HOCN/CNT-based TENG delivers a maximum output of 365 nA and 5.32 V (3 Hz, 4 & times; 4 cm2) and functions reliably as a pressure sensor, with voltage response proportional to finger pressure and stable performance over 10,000 cycles. By addressing the longstanding processing and performance challenges of vegetable oil polymers, this study demonstrates the potential of biobased HOCN/CNT composites for self-powered sensing systems and sustainable energy applications.
The development of sustainable, high-performance bio-adhesives to replace formaldehyde-based resins remains a critical challenge for the wood industry. However, the low water resistance, poor penetration, and weak adhesion strength severely bottleneck the practical application of bio-adhesives. Here, we present a strong, tough, and flame-retardant soybean meal (SM)-based adhesive with high penetration through a hierarchical dual bio-inspired strategy, combining the hard-soft phase combination of bivalve hinges and the root-like topological entanglement of plants. In this system, calcium sulfoaluminate (CSA) acts as rigid fillers to prompt crack deflection and energy dissipation, while polyacrylamide (PAM) entanglement further enhances the toughness of the SM matrix and mechanical interlocking at the interface. The prepared SM-adhesive achieves significant enhancements in dry shear strengths and wet work of adhesive, which were 6.0 folds and 37.5 folds higher than those of the primary SM. Furthermore, prepared adhesive exhibits excellent flame retardancy with limiting oxygen index of 32.5%, attributing to the gas-phase protective layer and condensed-phase flame retardancy of CSA. This work establishes a sustainable pathway for replacing traditional petroleum-based adhesives in plywood, and it has potential to develop on industrial-scale and achieve eco-friendly alternatives in the future.
Eutectic gels as important conductive polymers have promising practical applications in wearable electronic devices. However, the development of the ultra-stretchable and self-adhesive eutectic gel for multifunctional flexible sensors remains a challenge. Here, a lignin-enabled ultra-stretchable eutectic gel (LEG) integrating with excellent self-adhesion and high conductivity is prepared through polymerizable deep eutectic solvents (PDES) treated lignin followed by in-situ polymerization. In this LEG, the lignin macromolecules are utilized as important mediators to build dynamic crosslinking points in the polyacrylic acid (PAA) networks via hydrogen bond interactions. The dynamic disruption and reconstruction of the hydrogen bonds between the mobile PAA chain and dynamic crosslinking points ensure the high integrity of the crosslinking network to realize the ultra-stretchability (about 4845 %). Additionally, the abundant phenol groups of lignin endow the LEG with robust self-adhesion, which allows the LEG to seamlessly adhere to the different substrates. Based on these features, the LEGs are assembled as wearable strain sensors with high sensitivity, fast response time, and long-term sensing stability, and this wearable strain sensor demonstrates promising applications in human motion monitoring and information encryption systems. This work develops an effective pathway to design lignin-enabled ultra-stretchable eutectic gels for multifunctional sensors.
Self-powered electronic textiles undergo repeated deformation and friction, which imposes higher demands on the mechanical durability and sustainability of the dielectric polymeric substrates. However, designing the ideal polymeric substrates simultaneously possessing high strength and toughness, and excellent reprocessing performance for highly durable electronic textiles remains a rigorous challenge due to the intrinsic conflict in the mechanisms. Herein, we present a design concept that cellulose-enabled reversible chemical micro-crosslinking combination with multiple hierarchical hydrogen bonds induced dynamic crosslinking microdomains to realize the superior strength and toughness, and reprocessable bio-elastomers. The disintegration of hierarchical hydrogen bonds dissipating energy combination with the orientation arrangement of dynamic crosslinking microdomains along the stretching direction miraculously realize the superior mechanical strength (55.58 MPa) and toughness (144.25 MJ/m3). The reversible breakage and reconstruction of the dynamic crosslinking microdomains allow the bio-elastomer to be reprocessed for several cycles with extremely high mechanical strength recovery efficiency of 91.54 %. The bio-elastomers are employed as dielectric layers to laminate with the PPy-modified cotton fabric for large-scale manufacture of TENG-based electronic textiles with high stability, durability, and washability. The application scenarios are demonstrated for energy harvesting, motion monitoring, and human-computer interaction, providing a novel paradigm for environmental friendliness and durable wearable electronics.
ABSTRACT Selective CO 2 photoreduction via artificial photocatalysis into high‐value chemical feedstocks such as CO is a productive strategy for remitting environmental problems and energy crises. Nevertheless, photocatalysts generally endure low activity and poor product selectivity due to the low light/CO 2 capture and slow dynamic transfer of photogenerated electrons. Herein, we describe an all‐in‐one lignin‐based artificial thylakoid nanovesicle (AiO‐L‐ATN) using the confined growth strategy of lignin molecules, inspired by the chloroplast's photosynthesis mechanism. Such AiO‐L‐ATN possesses a high CO generation rate of 98.8 μmol g −1 h −1 at normalized active mass with a satisfactory selectivity of 92.1% in a gas‐solid system with H 2 O, exceeding 26 times that of the primary ZnCdS. Besides, introducing carbon nanovesicles significantly improves CO 2 capture performance, narrows the band gap, expands the wavelength range of light absorption, and accelerates the separation of photogenerated electrons. Density functional theory (DFT) calculation reveals that the carbon nanovesicles with various functional groups favor *CO 2 adsorption, *COOH production and conversion, as well as accelerate the dynamic transfer of photogenerated electrons, thereby endowing the outstanding CO 2 reduction rate and CO selectivity of AiO‐L‐ATN. This study not only provides valuable insights into the preparation of highly efficient photocatalysts but also offers novel avenues for CO 2 photoreduction.