Caichao Ye

The core bottleneck in photocatalytic CO ₂ reduction toward multi‐carbon oxygenates lies in the thermodynamic‐kinetic dual limitations of the C–C coupling step. Conventional strategies have focused on intrinsic electronic structure optimization of active sites while overlooking the critical influence of the reaction microenvironment on coupling probability. Herein, we propose a dynamic soft‐confinement catalytic strategy by in situ constructing a disordered hydrogen‐bonded organic framework (HOF) layer on Bi ₃ O ₄ Br surfaces, thereby establishing an HOF/Bi ₃ O ₄ Br integrated photocatalytic system. The introduction of HOF not only induces the formation of asymmetric Bi ₁ –Bi ₂ coupling sites but also establishes a dynamic hydrogen‐bonding microenvironment surrounding them. This microenvironment enhances CO ₂ coverage near the coupling sites by constructing a persistent carbon source enrichment layer. Simultaneously, the interfacial polarization field promotes exciton dissociation and directs electron transport toward the Bi ₁ –Bi ₂ sites. Furthermore, the reconfigurable hydrogen bonds impose orientational soft confinement on *CO intermediates, guiding them into spatial configurations favorable for *OCCO bond formation. This soft‐hard synergistic interfacial design enables 0.7HOF/Bi ₃ O ₄ Br to achieve a CH ₃ COOH production rate of 325.12 µmol g ⁻¹ h ⁻¹ with 98.81% product selectivity under sacrificial agent‐free conditions. This work demonstrates that dynamic microenvironment programming around active sites constitutes a critical pathway for overcoming the photocatalytic C–C coupling bottleneck.

The core bottleneck in photocatalytic CO ₂ reduction toward multi‐carbon oxygenates lies in the thermodynamic‐kinetic dual limitations of the C–C coupling step. Conventional strategies have focused on intrinsic electronic structure optimization of active sites while overlooking the critical influence of the reaction microenvironment on coupling probability. Herein, we propose a dynamic soft‐confinement catalytic strategy by in situ constructing a disordered hydrogen‐bonded organic framework (HOF) layer on Bi ₃ O ₄ Br surfaces, thereby establishing an HOF/Bi ₃ O ₄ Br integrated photocatalytic system. The introduction of HOF not only induces the formation of asymmetric Bi ₁ –Bi ₂ coupling sites but also establishes a dynamic hydrogen‐bonding microenvironment surrounding them. This microenvironment enhances CO ₂ coverage near the coupling sites by constructing a persistent carbon source enrichment layer. Simultaneously, the interfacial polarization field promotes exciton dissociation and directs electron transport toward the Bi ₁ –Bi ₂ sites. Furthermore, the reconfigurable hydrogen bonds impose orientational soft confinement on *CO intermediates, guiding them into spatial configurations favorable for *OCCO bond formation. This soft‐hard synergistic interfacial design enables 0.7HOF/Bi ₃ O ₄ Br to achieve a CH ₃ COOH production rate of 325.12 µmol g ⁻¹ h ⁻¹ with 98.81% product selectivity under sacrificial agent‐free conditions. This work demonstrates that dynamic microenvironment programming around active sites constitutes a critical pathway for overcoming the photocatalytic C–C coupling bottleneck.

Key Points: SLCO4A1 regulated PGE ₂ -mediated sodium transport by modulating E-prostanoid receptor activation and renal sodium transporter expression. Renal tubular SLCO4A1 deficiency increased interstitial PGE ₂ accumulation and promoted natriuresis and diuresis. Background: Renal sodium retention is a central driver of hypertension and fluid overload. PGE ₂ has long been identified as a potent natriuretic and diuretic factor. However, the mechanisms governing intrarenal PGE ₂ signaling and tubular sodium transport remain incompletely understood. Methods: Global and renal tubule–specific Slco4a1 knockout mouse, as well as renal tubule–specific Slco4a1 overexpressing mice, were generated to investigate the role of SLCO4A1 in renal sodium and water homeostasis. Computational docking, cellular studies, and in vivo functional analyses were performed to evaluate the role of SLCO4A1 in intrarenal distribution of PGE ₂ and its effect on tubular sodium transport. Results: SLCO4A1 was predominantly localized to the basolateral membrane of multiple renal tubular epithelial cells. Global and renal tubule–specific Slco4a1 gene deletion increased urine output and sodium excretion and reduced sodium reabsorption across multiple nephron segments in mice. This was accompanied by downregulation of key sodium transporters and channels, including sodium-glucose cotransporter 2, sodium-hydrogen exchanger 3, Na⁺-K⁺-2Cl⁻ cotransporter 2, sodium-chloride cotransporter, and epithelial sodium channel (ENaC). By contrast, renal tubule–specific overexpression of Slco4a1 displayed an opposite effect. Mechanistically, Slco4a1 deficiency led to accumulation of PGE ₂ in the kidney interstitium, which suppressed the expression of sodium transporter and channels through the E-prostanoid (EP) receptors. Specifically, EP ₁ mediated the PGE ₂ -induced suppression of Na⁺-K⁺-2Cl⁻ cotransporter 2, α -ENaC, and β -ENaC. EP ₂ was responsible for the suppression of sodium-chloride cotransporter, while EP ₃ was involved in suppressing sodium-glucose cotransporter 2, sodium-hydrogen exchanger 3, and γ -ENaC. Conclusions: Collectively, these findings uncovered a previously unrecognized role of SLCO4A1 in regulating intrarenal PGE ₂ distribution and identified SLCO4A1–PGE ₂ –EP receptor axis in fine-tuning renal tubular sodium transport.

The commercialization of aqueous zinc–metal batteries (AZMBs) is hindered by dendrite growth caused by uncontrolled Zn ²⁺ transport and side reactions involving water and anions. Here, an angstrom–scale confined ion sieve and accelerator is designed using unilamellar Ti _0.87 O ₂ nanosheets with atomic Ti vacancies (∼3.0 × 3.8 Å) and interlayer spacing (∼3.5 Å) to enable selective Zn ²⁺ (∼1.5 Å) transport while blocking H ₂ O (∼4.0 Å) and SO ₄ ²⁻ (∼5.9 Å). This design facilitates selective Zn ²⁺ ion transport with high flux and Zn/SO ₄ ²⁻ selectivity, effectively mitigating water–/anion–induced parasitic reactions at the Zn anode. Consequently, the Ti _0.87 O ₂ @Zn anode exhibits significantly suppressed dendrite growth and parasitic side reactions during repeated Zn plating/stripping, with stable cycle lives exceeding 5000 and 4000 h at 1 and 5 mA cm ⁻² , respectively. The Ah–level Ti _0.87 O ₂ @Zn//VO ₂ pouch cell retains 85.4% of its initial capacity after 300 cycles at 3 A g ⁻¹ . This strategy provides a promising interfacial design concept for improving the reversibility of aqueous Zn metal anodes and may inspire the rational design of confined ion–transport interphases for related aqueous battery systems.

Direct solar‐driven conversion of CO ₂ and H ₂ O into high‐value‐added C ₂ products, such as acetic acid, represents a critical frontier challenge in artificial photosynthesis. However, its efficiency is primarily constrained by sluggish photogenerated charge migration and the dynamics limitations for C‐C coupling. This paper reports a “disorder‐induced reconstruction” strategy that utilizes the inherent local disorder of covalent organic frameworks (COFs) to induce the construction of asymmetric active centers on the surface of Bi ₂₄ O ₃₁ Br ₁₀ (BOB), inducing atomic‐scale reconstruction and spontaneously forming extended regions with asymmetric Bi(δ+)‐Bi(δ‐) bimetallic sites. Without the use of sacrificial agents or noble metal co‐catalysts, the resulting catalyst exhibits excellent performance in the conversion of CO ₂ to acetate, with a yield as high as 1.03 mmol g ⁻¹ h ⁻¹ and a selectivity of 97.63%. The apparent quantum efficiencies of catalyst can reach 13.75% and 8.33% at 380 and 400 nm, respectively. This work reveals a previously unknown mechanism for reconstructing inorganic surfaces into asymmetric active structural units using local disorder in organic modifiers, providing a paradigm for the design of next‐generation photocatalysts.

Delta manganese dioxide (δ‐MnO ₂ ) has been extensively investigated as an attractive cathode material for aqueous zinc‐ion batteries (AZIBs) owing to its large interlayer spacing that facilitates ion storage and transport. However, the random restacking of 2D MnO ₂ nanosheets significantly limits their accessible surface area and increases diffusion resistance, thereby severely degrading electrochemical performance. Herein, we report a scalable synthesis of 3D structured aerogels from defect‐rich MnO ₂ nanosheets via a divalent metal ion‐initiated self‐assembly process for durable aqueous zinc‐ion batteries. The addition of metal ions enables MnO ₂ nanosheets in solution to assemble into a 3D network by neutralizing electrostatic repulsion and serving as intersheet linkers. The obtained 3D Mn vacancy‐rich MnO ₂ aerogel (A‐MnO ₂ ) cathode demonstrate greatly enhanced electrochemical performance, especially superior rate performance (146.3 mAh g ⁻¹ at 5 A g ⁻¹ ), and long‐term cycling stability (90.6% capacity retention after 5000 cycles at 5 A g ⁻¹ ). Moreover, the experimental analysis and theoretical calculations reveal that A‐MnO ₂ delivers improved conductivity, fast reaction kinetics, and superior structural stability, owing to abundant Mn vacancies and a 3D porous structure. This work may provide new insight for guiding the structural design of 2D electrode materials in AZIBs.

High‐performance polarized photodetectors (PDs) are crucial for image sensing and intelligent processing. Conventional detectors utilize multiple optical components, leading to complex systems that require advanced nanofabrication and customized micro‐nanostructures. This study presents a high‐performance polarization‐dependent PD utilizing the optical anisotropy and nanostructural features of three‐dimensional graphene (3D‐graphene) with a dual‐barrier modulation mechanism. The porous structure of 3D‐graphene allows differential light absorption based on incident direction, enhancing polarization selectivity, while its plasma resonator effect boosts localized electric fields. Incorporating tin dioxide quantum dots (SnO ₂ QDs) further improves polarization selectivity and carrier separation, reducing recombination losses. The device operates across a spectral range of 440–1550 nm, maintaining long‐term stability from 173 to 273 K. It features a detection rate of 1.21 × 10 ¹² Jones, a response rate of 21.18 A/W, low noise of 2.88 × 10 ⁻²⁰ A ² /Hz, and rise/fall times of 125 µs and 150 µs, respectively, with a cutoff frequency of 2.25 kHz. With a polarization ratio of 1.1, it is suited for polarization image processing and information encryption, achieving 99% recognition accuracy in detailed image reconstruction. This research provides valuable insights and foundational technical information for high‐performance polarized PDs.

Heterogeneous structured nanofluidic membranes show an extraordinary potential for selective ion transport. In particular, heterogeneous membranes with periodically asymmetric nanofluidic channels are expected to exhibit optimal ion selectivity, yet have rarely been achieved to date. Herein, we designed a two-dimensional (2D) organic–inorganic superlattice-like membrane with periodically arranged molecular-level asymmetric channels that achieve high iodide-ion selectivity and permeability. The PDDA/Ti_0.87O₂ superlattice-like membranes (PDDA/Ti_0.87O₂ SLMs) were prepared from unilamellar Ti_0.87O₂ nanosheets with surface-modified poly(diallyldimethylammonium chloride) (PDDA) by a layer-by-layer assembly strategy, in which the PDDA layers and Ti_0.87O₂ nanosheets are alternatively stacked to form molecular-level asymmetric channels between the heterogeneous units periodically. Unlike conventional nonperiodic structures with discontinuous ion migration paths and high ion-diffusion resistance, superlattice-like membranes provide continuous, unobstructed transport channels, enabling I^– ions to follow a periodic adsorption–repulsion synergistic transport mechanism, thereby forming nearly frictionless continuous ionic flow. As a result, the PDDA/Ti_0.87O₂ SLMs produce a record I^–/SO₄^2– selectivity of ∼680, which is the highest among all reported materials. When applied to osmotic energy generators with the artificial iodine wastewater, the PDDA/Ti_0.87O₂ SLMs can facilitate sustainable osmotic power generation and maintain operation for at least 160 h. In addition, the resulting iodine solution can be effectively utilized as a sterilizing agent with a high bactericidal effect of 99.5% for Escherichia coli within 30 min. This study establishes a new paradigm for periodic molecular-level asymmetric channels, presenting an approach for maximizing resource utilization from industrial iodine wastewater.

High-entropy oxides have emerged as a promising group of candidates for various catalytic fields, including seawater electrolysis. However, without rational understanding and guidance, designing multielement compositions for high-entropy systems and elucidating the synergistic effect of diverse elements in catalysis remain significant challenges. Herein, we report spin-state regulation of a high-entropy Ruddlesden-Popper perovskite oxide for efficient seawater electrolysis. The Cu²⁺ and Mn³⁺ with Jahn-Teller effect induced a transition of Fe³⁺/Co³⁺ spin state from low spin to high spin configuration. The high spin Fe³⁺/Co³⁺ favor OH^- adsorption and deprotonation during seawater oxidation. Besides, the oxygen intermediates adsorbed on high spin active sites repel the Cl^- ions. Consequently, (La_0.76Sr_0.24)₃(Fe_0.22Co_0.21Ni_0.18Cu_0.17Mn_0.22)₂O₇ achieved robust seawater oxidation for over 1200 h at 200 mA cm^-2, showing competitive performance. The anion exchange membrane electrolyzer coupling with (La_0.76Sr_0.24)₃(Fe_0.22Co_0.21Ni_0.18Cu_0.17Mn_0.22)₂O₇ anode and Pt/C cathode could maintain the seawater splitting performance of 1 A cm^-2 at 1.76 V and incessantly operate for 800 h. This spin-engineered strategy is universal to other high-entropy perovskite oxides and spinel oxides, offering promising way for designing efficient high-entropy catalysts.