Xiong Wen Lou

Encapsulating Hollow Perovskite Fluorides in Atomic Mn‐Embedded N‐Doped Carbon Fibers for Anode‐Less 5 V‐Class Li Metal Batteries

Demonstrates improved battery performance in anode-less lithium metal batteries, indicating potential for energy dense applications.

Ferrous Pyrophosphate Hollow Nanorods Enable Lithium Metal Batteries Under Low Negative/Positive Capacity Ratios

Shows improved capacity retention in lithium metal batteries using ferrous pyrophosphate nanorods, suggesting significant advancements in battery technologies.

Manufacturing‐Driven Programming of Carbon Interfaces via Controlled Densification for Solid‐State Sodium Storage

Demonstrates enhanced interfacial stability in solid-state sodium storage, suggesting controlled densification is beneficial.

Bromine-mediated electrochemical propane dehydrogenation by self-assembled ionic liquid-SnO ₂ hollow spheres

An electrocatalytic approach demonstrates efficient propane dehydrogenation, suggesting improved performance over conventional methods.

Synergistic Co‐Doping of Barium and Cobalt Enables Stable and Active RuO ₂ for Acidic Water Oxidation

Synergistic Co‐Doping of Barium and Cobalt Enables Stable and Active RuO ₂ for Acidic Water Oxidation

Demonstrates how co-doping barium and cobalt improves the stability and performance of electrocatalysts for hydrogen production.

Highly Active IrO x Formation on Strontium Manganite for Acidic Oxygen Evolution

Iridium-based oxides are considered the most effective catalysts for the acidic oxygen evolution reaction (OER) due to their superior stability and high activity. However, the high Ir content required poses a significant barrier to their commercial application. Enhancing OER activity and durability while simultaneously reducing the Ir loading remains a significant challenge. Here, porous strontium manganate nanofibers are synthesized via electrospinning and the element leaching behavior is exploited during hydrothermal synthesis to load short-range ordered IrOx with high activity. In situ characterizations, including X-ray absorption spectroscopy and Raman spectroscopy, confirm the structural stability of the short-range ordered IrOx during the OER process. Complementary theoretical calculations, differential electrochemical mass spectrometry, and in situ synchrotron-radiation infrared spectroscopy reveal that Mn suppresses the lattice oxygen mechanism, enabling the catalyst to stabilize OER through the adsorbate evolution mechanism. The synthesized low-Ir-loading catalyst exhibits high OER activity (221 mV overpotential at 10 mA cm⁻²) and robust stability (≈1000 h).

Fluorine Modified Zeolitic Imidazolate Framework Enables Long‐Life Zn–I₂ Batteries by Suppression of Polyiodide Shuttle

Modification using fluorine-containing zeolitic imidazolate frameworks inhibits the polyiodide shuttle effect, improving battery life.

Fluorine Modified Zeolitic Imidazolate Framework Enables Long‐Life Zn–I₂ Batteries by Suppression of Polyiodide Shuttle

Synthesis of H-F-ZIF nanoparticles suppresses the iodine shuttle effect, improving battery performance.

A functionalized porous Al current collector enables high-energy density anode-free Na batteries

The functionalized current collector improves energy density and stability in anode-free Na batteries, suggesting its potential for practical applications.

Efficient Cu─Co Dual‐Sites in Cobalt Oxide Nanoboxes for Electrocatalytic Reduction of Low‐Concentration NO to NH ₃

, highlighting a propitious direction for investigating highly efficient conversion of low-concentration NO exhaust gas.

Foldable anode-free sodium batteries enabled by N,P-codoped carbon macroporous fibers incorporated with CoP nanoparticles

Anode-free sodium batteries (AFNBs) are regarded as promising alternatives for next-generation energy storage systems because of their high energy density, high safety, cost-effectiveness, and simple manufacturing processes. However, their practical application is limited by a low coulombic efficiency (CE) and a short lifespan resulting from a large volume change and the growth of Na dendrites. Here, we propose a three-dimensional versatile host composed of interconnected N,P-codoped carbon macroporous fibers incorporated with CoP nanoparticles (denoted as CoP@N/P-CMFs) for selective nucleation and uniform deposition of Na. The porous skeleton reduces structural stress and inhibits dendrite growth by decreasing local current density and homogenizing Na + flux. Furthermore, the sodiophilic CoP and N,P-codoped carbon reduce the energy barrier for Na nucleation, further manipulating homogeneous Na growth. Consequently, the CoP@N/P-CMFs exhibit an ultrahigh CE of more than 99.97% (10 milliamperes per square centimeter and 10 milliampere-hours per square centimeter) and dendrite-free Na deposition. When coupled with a Na 3 V 2 (PO 4 ) 3 cathode, the assembled foldable AFNBs demonstrate stable cycling performance.

Surface Transformation in Lanthanum Nickelate for Enhanced Oxygen Evolution Catalysis

Nickel-based perovskite oxides are identified as promising candidates for oxygen evolution reaction (OER) catalysts in view of their low cost, highly tunable structure, and potential high activity. However, the performance and catalyst design are hindered by their sluggish surface reconstruction kinetics. We introduce a ferric ion pre-etching strategy to enhance the surface reconstruction of typical LaNiO₃. The hydrolysis of ferric ions generates hydrated protons that corrode the La-O terminal sites, inducing lattice distortion and lowering the energy barrier for reconstruction. Concurrently, ferric ion substitution for Ni creates crucial active sites after OER reconstruction, and enables the low-activity LaNiO₃ to become highly active and superior to the benchmark RuO₂ and NiFe layered double hydroxides (LDHs). In situ X-ray absorption spectroscopy (XAS) and in situ Raman spectroscopy reveal substantial surface transformation from corner-sharing to edge-sharing NiO₆ at 1.43 V versus reversible hydrogen electrode (RHE) in the surface pre-etched sample (LNFeIII-spe). This reconstruction is initiated by the lattice oxygen mechanism (LOM) and transitions to the adsorbate evolution mechanism (AEM), underscoring the transformation of distinct OER mechanisms.

Surface Transformation in Lanthanum Nickelate for Enhanced Oxygen Evolution Catalysis

Nickel‐based perovskite oxides are identified as promising candidates for oxygen evolution reaction (OER) catalysts in view of their low cost, highly tunable structure, and potential high activity. However, the performance and catalyst design are hindered by their sluggish surface reconstruction kinetics. We introduce a ferric ion pre‐etching strategy to enhance the surface reconstruction of typical LaNiO 3 . The hydrolysis of ferric ions generates hydrated protons that corrode the La‐O terminal sites, inducing lattice distortion and lowering the energy barrier for reconstruction. Concurrently, ferric ion substitution for Ni creates crucial active sites after OER reconstruction, and enables the low‐activity LaNiO 3 to become highly active and superior to the benchmark RuO 2 and NiFe layered double hydroxides (LDHs). In situ X‐ray absorption spectroscopy (XAS) and in situ Raman spectroscopy reveal substantial surface transformation from corner‐sharing to edge‐sharing NiO 6 at 1.43 V versus reversible hydrogen electrode (RHE) in the surface pre‐etched sample (LNFe III ‐ spe ). This reconstruction is initiated by the lattice oxygen mechanism (LOM) and transitions to the adsorbate evolution mechanism (AEM), underscoring the transformation of distinct OER mechanisms.

Regulating the Local Reaction Microenvironment at Chromium Metal–Organic Frameworks for Efficient H ₂ O ₂ Electrosynthesis in Neutral Electrolytes

The electrochemical synthesis of hydrogen peroxide represents a promising alternative to the traditional anthraquinone process, aiming for zero pollution. However, achieving efficient electrochemical synthesis of hydrogen peroxide in neutral electrolytes is challenging due to the sluggish kinetics of the two-electron oxygen reduction reaction. To address this issue, a unique metal-organic framework (MOF) featuring Cr metal sites coordinated with tetrabromoterephthalic acid (Cr-TBA) is synthesized. This specially designed MOF exhibits a distinctive paper-clip-like structure and remarkably enhanced Lewis acidity. Experimental results demonstrate that the obtained structure can facilitate the attraction of OH⁻ ions in solution, promoting their accumulation on the catalyst surface. This enhancement leads to excellent performances of Cr-TBA in neutral electrolytes, achieving Faradaic efficiencies of 96-98% and a production rate of 13.4 mol gcat ⁻¹ h⁻¹ at the current density of 150 mA cm⁻². Operando spectroscopy and density functional theory calculations indicate that this modified microenvironment effectively facilitates the conversion of the *OOH intermediates to H₂O₂ on the catalyst surface.

Electron‐Deficient Cobalt Centers Realized by Rational p─π Conjugation Regulation for High‐Performance Li─S Batteries

Rational design of the coordination environment of single‐atom catalysts (SACs) can enhance their catalytic activity, which is of great significance for high‐loading and lean‐electrolyte lithium‐sulfur (Li─S) batteries. Inspired by the Lewis acid–base theory, we design a unique coordination environment for constructing electron‐deficient Co SACs on carbon nanotubes (named as CNT@f‐CoNC), which function as a Lewis acid, to enhance the chemisorption and catalytic activity towards polysulfides (Lewis base). Compared with porphyrin‐like Co SACs, electron‐deficient Co SACs (Lewis acid) exhibit much stronger binding affinity towards polysulfides (Lewis base) and a significantly lower energy barrier of the rate‐determining step in the sulfur reduction reaction. As expected, even with a high sulfur loading (6.9 mg cm −2 ) and lean electrolyte to sulfur (E/S) ratio (4.0 µL mg −1 ), the areal capacity still reaches 7.7 mAh cm −2 . Moreover, a 1.6 Ah‐class pouch cell is successfully assembled under the harsh conditions and delivers an energy density of 422 Wh kg −1 . This work provides novel insights into enhancing the electrochemical performance of Li─S batteries by modulating the local electronic density of metal sites through the rational design of the coordination environment.

Electron‐Deficient Cobalt Centers Realized by Rational p─π Conjugation Regulation for High‐Performance Li─S Batteries

Rational design of the coordination environment of single‐atom catalysts (SACs) can enhance their catalytic activity, which is of great significance for high‐loading and lean‐electrolyte lithium‐sulfur (Li─S) batteries. Inspired by the Lewis acid–base theory, we design a unique coordination environment for constructing electron‐deficient Co SACs on carbon nanotubes (named as CNT@f‐CoNC), which function as a Lewis acid, to enhance the chemisorption and catalytic activity towards polysulfides (Lewis base). Compared with porphyrin‐like Co SACs, electron‐deficient Co SACs (Lewis acid) exhibit much stronger binding affinity towards polysulfides (Lewis base) and a significantly lower energy barrier of the rate‐determining step in the sulfur reduction reaction. As expected, even with a high sulfur loading (6.9 mg cm −2 ) and lean electrolyte to sulfur (E/S) ratio (4.0 µL mg −1 ), the areal capacity still reaches 7.7 mAh cm −2 . Moreover, a 1.6 Ah‐class pouch cell is successfully assembled under the harsh conditions and delivers an energy density of 422 Wh kg −1 . This work provides novel insights into enhancing the electrochemical performance of Li─S batteries by modulating the local electronic density of metal sites through the rational design of the coordination environment.

Operando unveiling the activity origin via preferential structural evolution in Ni-Fe (oxy)phosphides for efficient oxygen evolution

Non-noble metal-based heteroatom compounds demonstrate excellent electrocatalytic activity for the oxygen evolution reaction (OER). However, the origin of this activity, driven by structure evolution effects, remains unclear due to the lack of effective in situ/operando techniques. Herein, we employ the operando quick-scan x-ray absorption fine structure (Q-XAFS) technique coupled with in situ controlled electrochemical potential to establish a structure-activity correlation of the OER catalyst. Using Ni-Fe bimetallic phosphides as a model catalyst, operando Q-XAFS experiments reveal that the structural transformation initiates at the preferential oxidation of Fe sites over Ni sites. The in situ-generated O-Fe-P structure serves as the origin of the enhanced electrocatalytic OER activity of the catalyst, a finding supported by theoretical calculations. This work provides crucial insights into understanding the reaction mechanism of the state-of-the-art Ni-Fe-based OER electrocatalysts, thus advancing the rational design of more efficient OER electrocatalysts.

Oxygen‐Coordinated Single‐Atom Nickel Catalysts Derived from Water‐Induced Metal–Organic Framework Aerogel for Efficient Water Oxidation

Research on metal–organic framework (MOF) aerogels is relatively scarce, primarily constrained by the limited availability of synthetic methods. Herein, a water‐induced rapid conversion process of MOF powder to MOF aerogel is demonstrated, where the macroscopic transition is essentially due to the reassembly of microscopic constituent units and the rapid alteration of morphological structure. The derived catalyst possesses abundant holes left by the acid leaching process, leading to the high enrichment of O‐coordinated single‐atom Ni sites on the concomitant carbon edges. Consequently, such a catalyst exhibits excellent catalytic activity for oxygen evolution reaction (OER) in alkaline media, only requiring a low overpotential of 279 mV to drive the benchmark current density of 10 mA cm −2 . Density functional theory calculations further reveal the reduced OER energy barrier over the edge‐enriched O‐coordinated single‐atom Ni sites, as compared with internal O‐coordinated sites and traditional N‐coordinated sites. This is primarily attributed to the optimization effect of distinctive O‐coordinated structure and synergistic edge effect on the electronic structure of active Ni centers.

Oxygen‐Coordinated Single‐Atom Nickel Catalysts Derived from Water‐Induced Metal–Organic Framework Aerogel for Efficient Water Oxidation

Research on metal–organic framework (MOF) aerogels is relatively scarce, primarily constrained by the limited availability of synthetic methods. Herein, a water‐induced rapid conversion process of MOF powder to MOF aerogel is demonstrated, where the macroscopic transition is essentially due to the reassembly of microscopic constituent units and the rapid alteration of morphological structure. The derived catalyst possesses abundant holes left by the acid leaching process, leading to the high enrichment of O‐coordinated single‐atom Ni sites on the concomitant carbon edges. Consequently, such a catalyst exhibits excellent catalytic activity for oxygen evolution reaction (OER) in alkaline media, only requiring a low overpotential of 279 mV to drive the benchmark current density of 10 mA cm −2 . Density functional theory calculations further reveal the reduced OER energy barrier over the edge‐enriched O‐coordinated single‐atom Ni sites, as compared with internal O‐coordinated sites and traditional N‐coordinated sites. This is primarily attributed to the optimization effect of distinctive O‐coordinated structure and synergistic edge effect on the electronic structure of active Ni centers.