Shengzhong (Frank) Liu

Product selectivity in the electrochemical CO ₂ reduction reaction is strongly governed by the surface adsorption properties of reactant molecules and reaction intermediates. Using oxide‐derived copper as a model electrocatalyst, it is demonstrated that sulfur modification can redirect the CO ₂ reduction pathway from multicarbon products to formate by tuning the adsorption configuration of CO ₂ . Notably, this selectivity transition is highly sensitive to the concentration of sulfide ions (S ²⁻ ), with a pronounced influence even at a concentration as low as 1 μmol/L. By combining in‐situ spectroscopy characterizations, theoretical calculations of adsorbed CO ₂ reduction intermediates, and controlled CO electrolysis experiments, it is revealed that the introduction of S ²⁻ alters the adsorption mode of CO ₂ on the Cu surface from C‐site adsorption to O‐site adsorption, thus enabling the observed switch in product selectivity of CO ₂ reduction. This work provides a new perspective for understanding and steering the product selectivity of the electrochemical CO ₂ reduction reaction by engineering the adsorption configuration of key intermediates.

The rapid expansion of autonomous IoT networks and wearable electronics has intensified the demand for photo-rechargeable zinc-based batteries (PRZBBs). While realizing high overall energy conversion efficiency intrinsically relies on cathode materials capable of multi-electron transfer reactions, current literature largely treats the fundamental electrochemistry of aqueous zinc batteries and the macroscopic engineering of solar-integrated devices as isolated domains. This review bridges this critical gap, offering a unique positioning by establishing a unified analytical framework that directly links fundamental multi-electron redox mechanisms to the dynamic architectural requirements of PRZBBs. Moving beyond a conventional cataloging of material classes, we critically evaluate diverse cathode platforms, including transition metal oxides, Prussian blue analogues, organics, halogens, and sulfur. Our incremental contribution lies in decoupling how specific multi-step reaction kinetics, distinct voltage plateaus, and dominant charge carriers dictate solar cell coupling strategies, particularly concerning maximum power point matching and intermittent charging adaptability. Furthermore, we critically and systematically assess the practical bottlenecks of these chemistries, such as shuttle effects, kinetic limitations, and voltage hysteresis, that hinder scalable integration. Finally, we distill these insights into a prioritized, roadmap-oriented perspective, outlining the short- to long-term engineering and scientific milestones necessary to translate fundamental multi-electron zinc chemistry into next-generation, commercially viable self-powered technologies.

Ultra‐wide‐bandgap (UWBG) perovskite solar cells are critical for constructing high‐efficiency multi‐junction tandem devices, yet their performance is constrained by severe nonradiative recombination and disorder in phase growth arising from high bromine content. Here, we report a rational anion‐cation pairing strategy using thiocyanate‐based ionic liquids to simultaneously modulate crystallization kinetics and passivate multidimensional defects in 1.93 eV UWBG perovskites. By co‐introducing formamidinium thiocyanate (FASCN) and 1‐ethyl‐3‐methylimidazolium thiocyanate (EImSCN), we achieve synergistic effects: the pseudohalide SCN ⁻ fills halide vacancies and suppresses ion migration, FA ⁺ compensates for volatile loss during annealing, and EIm ⁺ coordinates with the Pb‐I framework while hydrogen‐bonding with FA ⁺ . This integrated approach prolongs the crystal growth window, enlarges grain size, releases residual tensile strain, and reduces trap density. The resulting inverted devices deliver a champion power conversion efficiency of 16.76% with an open‐circuit voltage of 1.41 V and an exceptional fill factor of 83.37%. Moreover, unencapsulated devices retain 95% of their initial efficiency after 1500 h storage in N ₂ , and large‐area modules (28.79 cm ² ) achieve 13.80% efficiency, demonstrating scalability. This work provides a molecular‐level design route to high‐quality UWBG perovskite for commercial perovskite‐based tandem photovoltaics.

Rational molecular engineering of the perovskite/hole transport layer interface offers a promising route to simultaneously address inefficient charge extraction, defect-mediated recombination, and lead leakage in CsPbI3–xBrx perovskite solar cells. Herein, we introduce 2,2′-dinitro-9,9′-spirobifluorene (DN-SBF) as an interfacial molecular bridge to tackle these challenges. DN-SBF optimizes energy level alignment, establishes π–π interactions, and forms exciplexes with Spiro-OMeTAD, thereby facilitating interfacial charge transport. Meanwhile, DN-SBF passivates undercoordinated Pb2+ through multiple coordination modes, including robust bidentate chelation formed by adjacent nitro groups, effectively passivating defects and suppressing non-radiative recombination. Importantly, multipoint coordination immobilizes leachable Pb2+, substantially mitigating lead leakage and improving film biocompatibility. As a result, DN-SBF-engineered CsPbI3–xBrx devices achieve a champion power conversion efficiency of 22.40% along with significantly enhanced operational and environmental stability. This work highlights the potential of versatile molecular bridges to concurrently enhance performance, stability, and eco-friendliness, which may contribute to the development of more sustainable perovskite photovoltaics.

Inorganic CsPbBr ₃ perovskite nanocrystals are promising photocatalysts for CO ₂ reduction because of their excellent optoelectronic properties.

Self-assembled molecules (SAMs) commonly employed in inverted perovskite solar cells (PSCs) are plagued by severe molecular aggregation that leads to non-uniform substrate coverage, consequently increased interfacial charge recombination and compromised operational stability. To overcome this limitation, we rationally design a novel SAM, (4-(2,7-bis(4-methoxyphenyl)-9,9-dimethylacridin-10(9H)-yl)butyl)phosphonic acid (MeO-PhAPA), featuring a structurally distorted backbone. The core structure of MeO-PhAPA integrates an sp3-hybridized carbon atom bonded to two methyl groups, which imposes pronounced molecular distortion that breaks molecular planarity and effectively suppresses deleterious π-π stacking. Additionally, the single-bond-linked two methoxyphenyl substituents further increase steric hindrance. This tailored molecular design robustly suppresses intermolecular aggregation of MeO-PhAPA, favoring the formation of a uniform, well-wetted amorphous thin film. Concurrently, MeO-PhAPA optimizes interfacial energy level alignment and delivers superior hole-extraction capability. Moreover, compared with the conventional MeO-4PACZ SAM, MeO-PhAPA facilitates the growth of high-quality perovskite films with larger grain sizes, lower defect density, and reduced bulk residual stress. Consequently, inverted PSCs incorporating MeO-PhAPA achieve a champion power conversion efficiency of 26.85% (certified 26.62%), markedly outperforming the control device based on MeO-4PACZ (24.12%). The optimized devices also demonstrate substantially enhanced stability under prolonged operational and thermal stresses.

All‐inorganic perovskites are promising photovoltaic materials for tandem cells owing to their suitable bandgaps and enhanced photothermal stability. However, inverted inorganic perovskite solar cells (PSCs) suffer from efficiency losses and poor operational stability primarily by iodide oxidation, which in turn induces ion migration and defect formation. Traditional defect‐healing processes are often irreversible and static, and selective reduction of iodine and oxidation of Pb ⁰ are hardly achievable simultaneously. Herein, we target surface halide oxidation and develop a regenerative interfacial passivation strategy via redox mediator to improve power conversion efficiency (PCE) and stability of inverted inorganic PSCs, by judiciously designing a thiol‐containing surface modifier 3‐mercaptopropionohydrazide (MPH). The reversible conversion between thiol and disulfide allows MPH as a self‐regenerating redox mediator, facilitating the removal of I ₂ and Pb ⁰ while suppressing iodide oxidation in a sustainable manner. Meanwhile, hydrazide group provides additional reduction capability, together with multiple coordination sites with undercoordinated Pb ^{2 +} and form hydrogen bonds with halides on perovskite surface, dramatically reducing defect density and inhibiting ion migration. Consequently, MPH‐treated devices achieve a champion PCE of 22.17% with a high open‐circuit voltage of 1.27 V, retaining 91.1% of its initial efficiency after 1100 h of maximum powerpoint tracking, substantially outperforming the control devices.

Developing a single electrolyte capable of simultaneously stabilizing Zn metal and chemically distinct cathodes remains a central challenge for aqueous zinc batteries. Here, a low-dose (25 mM) ionic-liquid additive, 1-allyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide ([AMMPyr][TFSI]), is introduced to orchestrate Zn2+ solvation and bidirectional electrode interphases through cooperative ion-pair chemistry. The [TFSI]− enters the primary Zn2+ solvation sheath, disrupts the bulk-water hydrogen-bond network, lowers the Zn2+ transport/desolvation barrier, and promotes an anion-derived organic-inorganic interphase that suppresses hydrogen evolution, corrosion, and dendritic deposition. Concurrently, [AMMPyr]+ preferentially adsorbs on cathode surfaces and associates with soluble polyiodides, thereby shielding sulfur conversion from water-induced parasitic reactions and restricting iodine shuttling. This cooperative mechanism enables reversible Zn plating/stripping and broad compatibility with multiple cathodes. Zn||S cells deliver an energy density of 518.8 Wh kg−1 and retain 86% capacity after 500 cycles at 5 A g−1. The strategy further enables Zn||I2 to operate for 20000 cycles, Zn||V2O5 to retain 163.8 mAh g−1 after 1000 cycles, and Zn||AC capacitors to maintain 88% capacity over 90000 cycles. Moreover, a Zn||S pouch cell integrated with a solar cell realizes an overall conversion efficiency of 7.1%. This work establishes ion-pair engineering as a broadly applicable route toward durable aqueous zinc batteries and photo-rechargeable devices.