High Exposure Of Active Sites Research Articles

Zinc Oxide Nanoclusters Encapsulated in MFI Zeolite as a Highly Stable Adsorbent for the Ultradeep Removal of Hydrogen Sulfide.

Often, trace impurities in a feed stream will cause failures in industrial applications. The efficient removal of such a trace impurity from industrial steams, however, is a daunting challenge due to the extremely small driving force for mass transfer. The issue lies in an activity-stability dilemma, that is, an ultrafine adsorbent that offers a high exposure of active sites is favorable for capturing species of a low concentration, but free-standing adsorptive species are susceptible to rapidly aggregating in working conditions, thus losing their intrinsic high activity. Confining ultrafine adsorbents in a porous matrix is a feasible solution to address this activity-stability dilemma. We herein demonstrate a proof of concept by encapsulating ZnO nanoclusters into a pure-silica MFI zeolite (ZnO@silicalite-1) for the ultradeep removal of H2S, a critical need in the purification of hydrogen for fuel cells. The Zn species and their interaction with silicalite-1 were thoroughly investigated by a collection of characterization techniques such as HADDF-STEM, UV-visible spectroscopy, DRIFTS, and 1H MAS NMR. The results show that the zeolite offers rich silanol defects, which enable the guest nanoclusters to be highly dispersed and anchored in the silicious matrix. The nanoclusters are present in two forms, Zn(OH)+ and ZnO, depending on the varying degrees of interaction with the silanol defects. The ultrafine nanoclusters exhibit an excellent desulfurization performance in terms of the adsorption rate and utilization. Furthermore, the ZnO@silicalite-1 adsorbents are remarkably stable against sintering at high temperatures, thus maintaining a high activity in multiple adsorption-regeneration cycles. The results demonstrate that the encapsulation of active metal oxide species into zeolite is a promising strategy to develop fast responsive and highly stable adsorbents for the ultradeep removal of trace impurities.

A Hierarchical Metal-Organic Framework Composite Aerogel Catalyst Containing Integrated Acid, Base, and Metal Sites for the One-Pot Catalytic Synthesis of Cyclic Carbonates.

Catalysis has played a decisive role in the development of unique chemical reactions to produce important chemicals. However, conventional stepwise synthetic routes that rely on individual catalysts to promote each step often suffer from ponderous processes for the isolation of intermediates that result in massive material losses and large economic expenditures. In addition, traditional powder forms of these catalysts suffer from poor processability and recoverability. Herein, we designed and prepared a hierarchical metal-organic framework (MOF) composite monolithic catalyst IL-Au@UiO-66-NH2/CMC that contains integrated acid (Zr4+), base (ionic liquid (IL)), and metal sites (Au nanoparticles (NPs)) to promote the one-pot preparation of cyclic carbonates from styrene derivatives and CO2. Highly dispersed Au NPs, IL 1-aminoethyl-3-methylimidazolium bromide ([C2NH2 MIM] [Br]), and MOF-positioned Lewis acid sites within this composite aerogel are separately responsible for catalyzing selective epoxidation of the styrene derivatives and the subsequent cycloaddition reaction of CO2 with intermediate styrene oxides. Importantly, inclusion of the imidazolium-based IL effectively modulates the size and chemical microenvironment of the Au NPs via electrostatic protection, leading to catalyst stability and its selective oxidation of styrene. Benefiting from the rapid mass transfer and high exposure of active sites within the pore-rich hierarchical nanostructure, IL-Au@UiO-66-NH2/CMC promotes high conversion (90.5%) of the styrene and selectivity (80.5%) for styrene carbonate (SC) formation in the one-pot process, a performance level that far exceeds those of related catalysts containing only Au NPs or IL (the selectivity of SC < 42%). Furthermore, the composite aerogel catalyst can be readily separated and recycled at least five times without a remarkable loss of activity and selectivity. The controllable integration of various active components in the hierarchical MOF composite aerogel herein should serve as the foundation for the design of multifunctional monolithic catalysts for other valuable tandem processes.

Enhancement of Carrier Migration by Monolayer MXene Structure in Ti3CN/TiO2 Heterojunction to Achieve Efficient Photothermal Synergistic Transformation of CO2

Carbon nitride MXene exhibits good metal conductivity, high photothermal conversion, carrier mobility, and high exposure of active sites, which makes it a promising co-catalyst for photothermal synergistic transformation of CO2. In this paper, Ti3CN/TiO2 heterojunction was constructed in situ using Ti3CN as TiO2 precursor to investigate the performance of Ti3CN MXene in photothermal synergistic transformation of CO2, and then the monolayer structure was utilized to enhance the interfacial charge transfer and improve the photothermal catalytic activity of Ti3CN. The catalysts were characterized by SEM, XRD, XPS, and UV-Vis DRS, and it was found the heterojunction constructed by monolayer MXene had a narrower bandgap and a higher carrier generation mobility, which, combined with the catalytic activity test, proved the single monolayer Ti3CN MXene had better photothermal synergistic conversion efficiency of CO2, and the heterojunction yield was 11.36 μmol·g−1·h−1 after layering, compared with that before layering (9.41%), which was 1.2 times higher than that before layering (9.41 μmol·g−1·h−1).

Excellent Mercury Removal in High Sulfur Atmosphere Using a Novel CuS-BDC-2D Derived by Metal-Organic Frame.

To effectively remove high concentrations of mercury in a high sulfur atmosphere of nonferrous smelting flue gas, a novel two-dimensional CuS-MOF (CuS-BDC-2D) material is synthesized by anchoring S to Cu sites in the Cu-BDC MOF. The highly dispersed CuS active sites and MOF framework structural properties in CuS-BDC-2D enable efficiently collaborate in capturing mercury. CuS-BDC-2D exhibits a layered floral structure with high specific surface area and thermal stability, with poor crystallinity. Compared to CuS and the three-dimensional CuS-MOF (CuS-BDC-3D) structure, CuS-BDC-2D demonstrates significantly higher mercury capture capacity due to the high exposure of active sites and defects sites in the two-dimensional material. Moreover, CuS-BDC-2D exhibits excellent resistance to sulfur, maintaining its high efficiency in removing Hg0 even at high levels of sulfur dioxide (SO2), such as 5000-20,000 ppm. The superior performance of CuS-BDC-2D makes it suitable for controlling mercury emissions in actual nonferrous smelting flue gas. This discovery also paves the way for the development of new mercury adsorbents, which can guide future advancements in this field.

Self–Supporting Mn–RuO2 Nanoarrays for Stable Oxygen Evolution Reaction in Acid

Currently, the process of an acidic oxygen evolution reaction (OER) necessitates the use of Iridium dioxygen (IrO2), which is both expensive and incredibly scarce on Earth. Ruthenium dioxygen (RuO2) offers high activity for acidic OERs and presents a potential substitution for IrO2. Nevertheless, its practical application is hindered by its relatively poor stability. In this study, we have developed Mn–doped RuO2 (Mn–RuO2) nanoarrays that are anchored on a titanium (Ti) mesh utilizing a two–step methodology involving the preparation of MnO2 nanoarrays followed by a subsequent Ru exchange and annealing process. By precisely optimizing the annealing temperature, we have managed to attain a remarkably low overpotential of 217 mV at 10 mA cm−2 in a 0.5 M H2SO4 solution. The enhanced catalytic activity of our Mn–RuO2 nanoarrays can be attributed to the electronic modification brought about by the high exposure of active sites, Mn dopant, efficient mass transfer, as well as the efficient transfer of electrons between the Ti mesh and the catalyst arrays. Furthermore, these self–supported Mn–RuO2 nanoarrays demonstrated excellent long–term stability throughout a chronoamperometry test lasting for 100 h, with no discernible changes observed in the Ru chemical states.

Amorphous quaternary alloy nanoplates for efficient catalysis of hydrogen evolution reaction

Developing a highly efficient non-precious transition metal-based electrocatalyst via a facile approach toward the hydrogen evolution reaction (HER) is critical for large-scale hydrogen production but still remains challenging. Herein, a cost-effective electrochemical deposition strategy is rationally proposed to construct amorphous quaternary FeCoNiCu alloy nanosheets supported on nickel foam (NF) towards this challenge. Benefiting from the synergistic effect of multi-metal atoms interaction and the high exposure of active sites caused by abundant open voids, the as-synthesized FeCoNiCu/NF electrode exhibits high catalytic activity and robustness toward HER in alkaline solution, requiring an overpotential of only 35 mV to reach a current density of 10 mA cm–2. This study may pave a new avenue to design advanced electrocatalyst for energy conversion.

Tofukasu-derived biochar with interconnected and hierarchical pores for high efficient removal of Cr (VI)

Herein, we report the synthesis of interconnected hierarchical pore biochar (HTB) via an ice-templating strategy using bio-waste (tofukasu). The abundance of N- and O-containing functional groups in tofukasu makes it easy to form hydrogen bonds with water molecules and water clusters, resulting in nano-micro structures like ice clusters and snow crystals during freezing process. More importantly, tofukasu will be squeezed by micron-scale snow crystals to form coiled sheet-like structures, and its surface and interior will be affected by needle-like ice nanocrystals from several nanometers to tens of nanometers to form transverse groove needles and mesopores. The ice crystals are then removed by sublimation with tofukasu, leaving the interconnected pore structure intact. Therefore, the ice template synthesis strategy endowed the interconnected hierarchical pore structure of HTB with a large specific surface area (SBET, 733 m2⋅g−1) and hierarchical porosity (30.30% for mesopores/total pore volume ratio), which is significantly higher than the normal dry treated tofukasu biochar (TB), which had a SBET of 436 m2⋅g−1 and contained 1.53% mesopores. In addition, the sheet-like structure with interconnected pores of HTB favors high exposure of active sites (N- and O-containing functional groups), and a fast electron transport rate. As a result, HTB had an excellent adsorption capacity of 159.65 mg⋅g−1, which is 4.7 times that of typical block biochar of TB (33.89 mg⋅g−1) according to Langmuir model. Electrochemical characterization, FTIR and XPS analysis showed that the mechanism of Cr(VI) removal by HTB included electrostatic attraction, pore filling, reduction and surface complexation.Graphical

Monolithic-structured nickel silicide electrocatalyst for bifunctionally efficient overall water splitting

The rational design and synthesis of cost-effective and efficient bifunctional electrocatalysts are crucial for developing hydrogen energy yet challenging. Here we report porous monolith electrocatalysts (PMECs) comprising transition metal silicide (e.g., nickel silicide) with high activity and durability. These PMECs offer strong synergetic effects and high exposure of active sites, resulting in excellent kinetics in catalyzing both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), which surpass the benchmark catalysts RuO2 and Pt/C. The doping strategy is demonstrated to further enhance electrocatalytic performance by constructing Mo-doped Ni2Si PMEC, which requires only a cell voltage of 1.60 V at 100 mA cm−2. Density functional theory calculations display that the synergistic effect of Ni and Si can reduce the energy barriers of intermediate adsorption, and the introduction of Mo into Ni2Si can further decrease the energy barrier of determining step and optimize the H* adsorption energy, thus enhancing the electrochemical kinetics for OER and HER. Our work paves the way for designing high-efficiency and low-cost porous monolith catalysts through a facile and scalable method, showing great prospects for industrialization.

Surface-structure tailoring of Dendritic PtCo nanowires for efficient oxygen reduction reaction

Platinum-based alloy nanowire catalysts demonstrates great promise as electrocatalysts to facilitate the cathodic oxygen reduction reaction (ORR) of proton exchange membrane fuel cells (PEMFCs). However, it is still challenge to further improve the Pt atom utilization of Pt based nanowires featuring inherent structural stability. Herein, a new structure of PtCo nanowire with nanodendrites was developed using CO-assistance solvent thermal method. The dendrite structure with an average length of about 7 nm are characterized by a Pt-rich surface and the high-index facets of {533}, {331} and {311}, and grows from the ultra-fine wire structure with an average diameter of about 3 nm. PtCo nanowires with nanodendrites developed in this work shows outstanding performance for ORR, in which its mass activity of 1.036 A/mgPt is 5.76 times, 1.74 times higher than that of commercial Pt/C (0.180 A/mgPt) and PtCo nanowires without nanodendrites (0.595 A/mgPt), and its mass activity loss is only 18% under the accelerated durability tests (ADTs) for 5k cycles. The significant improvement is attributed to high exposure of active sites induced by the dendrite structure with Pt-rich surface with the high-index facets and Pt-rich surface. This structure may provide a new idea for developing novel 1D Pt based electrocatalysts.

Exchanging Anion in CuCo-Carbonate Double Hydroxide for Faradaic Supercapacitors: A Case Study.

A systematic synthetic method involving the anion exchange process was designed and developed to fabricate the superior functioning three-dimensional (3-D) urchin-architectured copper cobalt oxide (CuCo2O4; CCO) and copper cobalt sulfide (CuCo2S4; CCS) electrode materials from copper-cobalt carbonate double hydroxide [(CuCo)2(CO3)(OH)2; CCH]. The effective tuning of chemical, crystalline, and morphological properties was achieved during the derivatization process of CCH, based on the anion exchange effect and phase transformation without altering the 3-D spatial assembly. Benefiting from morphological and structural advantages, CCO and CCS exhibited superior electrochemical activity with capacity values of 1508 and 2502 C g-1 at 10 A g-1 to CCH (1182 C g-1 at 10 A g-1). The thermal treatment of CCH has generated a highly porous nature in nanospikes of 3-D urchin CCO structures, which purveys betterment in electrochemical phenomena than pristine smooth-surfaced CCH. Meanwhile, the sulfurization reaction induced the anion effect to a greater extent in the CCS morphology, resulting in hierarchical 3-D urchins formed by 1-D nanospikes constituting coaxially swirled 2-D nanosheets with high exposure of active sites, specific surface areas, and 3-D electron/ion transportation channels. The asymmetric supercapacitor was constructed with a superior CCS electrode as a cathode and an activated carbon electrode as an anode, showing a high specific capacity of 287.35 C g-1 at 7 A g-1 and durability for 5000 cycles with 94.2% retention at a high current density of 30 A g-1. The ultrahigh energy and power density of 135.3 W h kg-1 (10 A g-1) and 44.35 kW kg-1 (30 A g-1) were harvested during the PC device performance. Our finding proposes an idea about the importance of anions and phase transformation as a versatile tool for engineering high-functioning electrode materials and their endeavor toward overwhelming the major demerit of SCs by aggrandizing the energy density value and rate performance.

A series of crumpled ball-like metal oxide-based catalysts enabled by aerosol synthesis

Two-dimensional nano metal oxides (2D-NMOs) have attracted great concerns due to high exposure of active sites and short ion transport distance. However, 2D-NMOs with the layered structure render to restack into bulk ones, resulting in the active-sites coverage and ion-transport blockage. Here, crumpled 2D NMOs with paper-ball-like shape was proposed to avoid the restacking. Our new strategy can convert diversity of metal oxide into paper-ball-like structure with controllable composition by overcoming the fragile nature of metal oxide and limitation of growth pattern. Resultantly, as-prepared 2D NMOs demonstrated superior catalytic activity and durability in both oxygen evolution reaction (OER) and organic dye degradation reaction, owing to their high exposure of active sites and low ionic diffusion resistance.

A Kinetic Control Strategy for One‐Pot Synthesis of Efficient Bimetallic Metal‐Organic Framework/Layered Double Hydroxide Heterojunction Oxygen Evolution Electrocatalysts

AbstractHeterojunction materials are promising candidates for oxygen evolution reaction (OER) electrocatalysts to break the linear scaling relationship and lower the reaction barrier. However, the application of heterojunction materials is always hindered by the complicated multistep synthetic procedures which bring cost, complexity, and reproducibility issues. Herein, a strategy of kinetic controlled synthesis is developed to achieve the one‐pot formation of bimetallic metal‐organic framework (MOF)/layered double hydroxide (LDH) heterojunction electrodes as highly efficient OER electrocatalysts. The heterojunction electrodes present hierarchical structures with highly porous NiFe‐LDH nanosheet networks vertically grown on the surface of NiFe‐MOF‐74 microprisms, promoting fast mass transport and high exposure of active sites. The strong interactions at the MOF/LDH heterojunction interfaces contribute to the outstanding OER activity surpassing the state‐of‐art RuO2 OER catalysts. The MOF/LDH heterojunction electrode exhibits an ultralow overpotential of only 159.7 mV to reach the current density of 10 mA cm−2, and yields large current densities at small overpotential (100 mA cm−2 at 230.2 mV and 1000 mA cm−2 at 284.3 mV) with long‐term durability. This study presents an innovative approach to construct heterojunction materials with simple one‐step synthesis, offering a promising pathway for high‐efficiency electrocatalyst development.

Design of B, P co-doped CoNi bimetallic for boosting supercapacitor performance: Effect of boronation and phosphorization order

The exploration of high-efficiency electrodes is urgent for energy conversion and storage devices. In this work, CoNiBP nanosheets were fabricated by a successive method which is facile and cost-effective. The nanosheet-like structure of CoNiBP enables high exposure of active sites and fast transport of ions and electrons. In addition, the synergistic effect of B and P strengthens the electrochemical performance by tuning the electronic structure of active sites. The CoNiBP electrode exhibits a high specific capacity of 870.8 C g−1 at 1 A g−1 with excellent rate capability and stability. Moreover, the assembled CoNiBP//AC asymmetric supercapacitor (ASC) device delivered an ultrahigh energy density of 71.7 Wh kg−1 at 0.8 kW·kg−1 with good cyclability (∼100% retention of original capacity after 12 000 cycles). With such superior electrochemical performance, CoNiBP is a promising material to be used as electrode in supercapacitors.

Fabrication of the novel NiFe-LDHs @γ-MnOOH nanorod electrocatalyst for effective water oxidation

The development of highly efficient electrocatalysts for water splitting is great critical for the massive production of hydrogen energy. In this work, a kind of novel NiFe-LDHs@γ-MnOOH nanorod electrocatalyst was fabricated via the two-step method. Firstly, γ-MnOOH nanorods were grown in situ on the nickel foam conductive substrate by a simple hydrothermal method. Then, NiFe-LDHs were combined on the γ-MnOOH/NF surface by electrochemical deposition to prepare the NiFe-LDHs@γ-MnOOH/NF core-shell structure catalyst. Due to good charge transfer capability, high exposure of active sites as well as the interfacial interaction between NiFe-LDHs and γ-MnOOH, the obtained core-shell structure catalyst exhibited excellent oxygen evolution reaction (OER) activity in alkaline media. The overpotential of 226 mV at the current density of 10 mA cm−2 for OER could be achieved with a low Tafel slope of 88 mV dec- 1, and almost no current density loss occurred after the 24 h i-t stability testing. Furthermore, this catalyst also possessed good performance in overall water splitting, which could afford a current density of 10 mA cm−2 by 1.69 V cell voltage.

Two-Dimensional Metal-Organic Framework Superstructures from Ice-Templated Self-Assembly.

Here, we report the synthesis of two-dimensional (2D) layered metal-organic framework (MOF) nanoparticle (NP) superstructures via an ice-templating strategy. MOF NP monolayers and bilayers can be obtained by regulating the concentration of colloidal MOF NPs without any external fields during self-assembly. Adjacent polyhedral MOF NPs are packed and aligned through crystalline facets, resulting in the formation of a quasi-ordered array superstructure. The morphology of the MOF layers is well preserved when subjected to pyrolysis, and the obtained carbon NPs have hollow interiors driven by the outward contraction of MOF precursors during pyrolysis. With the advantages of large surface areas, hierarchical porosity, high exposure of active sites, and fast electron transport of the 2D layered structure, the mono- and bilayered carbon NP superstructures show better oxygen reduction activity than isolated carbon particles in alkaline media. Our work demonstrates that ice-templating is a powerful strategy to fabricate superstructures of various MOFs and their derivatives.

Well-dispersed ZIF-derived N-doped carbon nanoframes with anchored Ru nanoclusters as HER electrocatalysts

Nano-structuring and metal-support interactions are effective methods to improve the electrocatalytic activity of heterogeneous catalysis. In this study, we synthesized nitrogen-doped porous carbon substrates by using a SiO2-protected calcination strategy with ZIF-8 as a precursor. The experimental results revealed the prepared porous nitrogen-doped carbon (PNC) to have high dispersion, large specific surface area, and rich pore structure, allowing high exposure of active sites. The carbon support showed optimum characteristics to deposit precious metals with small particle sizes. X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) showed that the N groups on the PNC substrates served as coordination sites for Ru, allowing the formation of ultrafine nanoclusters. The Ru clusters showed good metal dispersion, exposing more active sites and improving the utilization of the precious metal. At a current density of 10 mA/cm2, Ru/PNC showed a minimum overpotential of 40 mV. This work provided a simple and effective method for the preparation of excellent carbon substrates and the synthesis of metal clusters with small particle sizes.

Mos2 Intercalated Mgcufe Layered Double Hydroxide: Activation of Peroxymonosulfate by High Exposure of Active Sites and Rapid Electron Transfer

Mos2 Intercalated Mgcufe Layered Double Hydroxide: Activation of Peroxymonosulfate by High Exposure of Active Sites and Rapid Electron Transfer

Defect-rich and ultrathin nitrogen-doped carbon nanosheets with enhanced peroxidase-like activity for the detection of urease activity and fluoride ion

Although carbon nanozymes have attracted great interest due to their good biocompatibility, low cost, and high stability, designing high-active carbon nanozymes still faces great challenges. Herein, ultrathin nitrogen-doped carbon nanosheets with rich defects (d-NC) were prepared through a high-temperature annealing process, using potassium chloride and ammonium chloride as templates. Owing to the large specific surface area, rich defects and the high exposure of active sites, the proposed d-NC nanozymes exhibited excellent peroxidase-like activity. The d-NC nanozymes possess maximal reaction velocity and their specific activity is 9.4-fold higher than that of nitrogen-doped carbon nanozymes, indicating that the induced defects can boost the catalytic performance. Benefited from the good peroxidase-like activities of d-NC nanozymes, the colorimetric sensing platforms were constructed for the detection of urease activity and fluoride ion, exhibiting satisfactory stability and selectivity. This study not only offers a way to synthesize carbon nanozymes with improved enzyme-like activities but also broadens their applications in colorimetric biosensing.

Engineering the coordination environment in atomic Fe/Ni dual-sites for efficient oxygen electrocatalysis in Zn-air and Mg-air batteries

Rational design the single atomic catalyst with excellent activity, stability and high exposure of active sites is a significant challenge. Here, we report an atomically dispersed iron and nickel co-anchored on defect-rich porous nitrogen and sulfur carbon frameworks (denoted as Fe, Ni-SAs/DNSC) with tailored coordination environment, The Fe, Ni-SAs/DNSC electrocatalyst displays outstanding catalytic activity for oxygen reduction reaction (ORR) with an onset potential (Eonset) of 1.03 V (vs. RHE), half-wave potential (E1/2) of 0.88 V (vs. RHE) as well as superior stability. The catalyst also shows a superior oxygen evolution reaction (OER) activity. When Fe, Ni-SAs/DNSC catalyst is employed as an air cathode, the Zn-air battery displays superior performance with a large peak power density of 160 mW cm−2, high energy density of 962.8 Wh kgZn-1 and cycling stability. Also, the Fe, Ni-SAs/DNSC-based liquid and flexible solid-state Mg-air batteries deliver a large peak power density of 76 mW cm−2, high energy density of 1653 Wh kgMg–1 and superior durability (Over 78 h at 20 mA cm−1). Furthermore, DFT calculations reveal that the doped S atom and carbon vacancy can weaken the binding strength between oxygen intermediates and Fe active site and improve the desorption of *OH step during the ORR process. This work provides insights into the design dual single atomic catalyst with a tailored coordination environment.

Laser‐Induced Annealing of Metal–Organic Frameworks on Conductive Substrates for Electrochemical Water Splitting

AbstractThe conventional thermal transformation of metal–organic frameworks (MOFs) for electrocatalysis requires high temperature, an inert atmosphere, and long duration that result in severe aggregation of metal particles and non‐uniform porous structures. Herein, a precise and inexpensive laser‐induced annealing (LIA) strategy, which eliminates particle aggregation and rapidly generates uniform structures with a high exposure of active sites, is introduced to carbonize MOFs on conductive substrates under ambient conditions within a few minutes. By systematically considering 8 substrates and 12 MOFs, a series of LIA‐MOF/substrate devices with controllable sizes and good flexibility are successfully obtained. These LIA‐MOF/substrate devices can directly serve as working electrodes. Remarkably, LIA‐MIL‐101(Fe) on nickel foam exhibits an ultralow overpotential of 225 mV at a current density of 50 mA cm−2 and excellent stability over 50 h for facilitating the oxygen evolution reaction, outperforming most recently reported transition‐metal‐based electrocatalysts and commercial RuO2. Physical characterizations and theoretical calculations evidence that the high activity of LIA‐MIL‐101(Fe) arises from the favorable adsorption of intermediates at its Ni‐doped Fe3O4 overlayer that is formed during the laser treatment. Moreover, the LIA‐MOF/substrate devices are assembled for overall water splitting. The proposed LIA strategy demonstrates a cost‐effective route for manufacturing scalable energy storage and conversion devices.