Sequence-controlled semiconducting polymers represent a new frontier in organic electronics, where precise molecular sequence directly dictates device performance. However, achieving both high sequence fidelity and structural diversity remains a significant challenge using conventional synthetic protocols. To address this issue, we introduce a versatile halide-pair-driven multicomponent polymerization (MCP) strategy that enables the library synthesis of sequence-controlled semiconducting poly(triarylamine)s (PTAAs). By optimizing halide pairing in conjunction with a rationally designed Buchwald ligand-Pd system featuring catalyst-transfer capability, we achieved efficient sequential cascade aminations, thereby enabling the MCP. The versatility of this strategy was demonstrated through the synthesis of a library of sequence-controlled PTAAs, including dendronized variants, underscoring its potential as a general platform for functional semiconducting material discovery.

Abstract Lithium (Li) metal, with its unparalleled theoretical capacity and lowest electrochemical potential, is a promising anode material for rechargeable batteries. Yet, challenges such as dendrite formation, severe electrode volume change, and ongoing Li consumption impede its practical adoption. To address these challenges, a novel approach is introduced, harnessing the switchable electrical conductivity of a nanoporous current collector for Li metal anode. A vertically aligned Nickel‐catecholate (VANC) is directly grown on the copper foil as the nanoporous current collector, and the Li intercalation and de‐intercalation of VANC reversibly decrease and increase the electrical conductivity in the direction perpendicular to the electrode, respectively. The switchable conductivity induces uniform deposition and stripping of Li metal without forming dendrite and dead Li during the Li plating/stripping process and thus enables high coulombic efficiency of over 98% even after 200 cycles. This nanoporous structure with switchable conductivity will open up a new path for reliable lithium metal anode for rechargeable battery applications.

Sequence-controlled semiconducting polymers represent a new frontier in organic electronics, where precise molecular sequence directly dictates device performance. However, achieving both high sequence fidelity and structural diversity remains a significant challenge using conventional synthetic protocols. To address this issue, we introduce a versatile halide-pair-driven multicomponent polymerization (MCP) strategy that enables the library synthesis of sequence-controlled semiconducting poly(triarylamine)s (PTAAs). By optimizing halide pairing in conjunction with a rationally designed Buchwald ligand-Pd system featuring catalyst-transfer capability, we achieved efficient sequential cascade aminations, thereby enabling the MCP. The versatility of this strategy was demonstrated through the synthesis of a library of sequence-controlled PTAAs, including dendronized variants, underscoring its potential as a general platform for functional semiconducting material discovery.

Abstract Lithium (Li) metal, with its unparalleled theoretical capacity and lowest electrochemical potential, is a promising anode material for rechargeable batteries. Yet, challenges such as dendrite formation, severe electrode volume change, and ongoing Li consumption impede its practical adoption. To address these challenges, a novel approach is introduced, harnessing the switchable electrical conductivity of a nanoporous current collector for Li metal anode. A vertically aligned Nickel‐catecholate (VANC) is directly grown on the copper foil as the nanoporous current collector, and the Li intercalation and de‐intercalation of VANC reversibly decrease and increase the electrical conductivity in the direction perpendicular to the electrode, respectively. The switchable conductivity induces uniform deposition and stripping of Li metal without forming dendrite and dead Li during the Li plating/stripping process and thus enables high coulombic efficiency of over 98% even after 200 cycles. This nanoporous structure with switchable conductivity will open up a new path for reliable lithium metal anode for rechargeable battery applications.

Precise control of multiple structural parameters associated with vinyl polymers is important for producing materials with the desired properties and functions. While the development of living polymerization methods has provided a way to control the various structural parameters of vinyl polymers, the concomitant control of their sequence and regioregularity remains a challenging task. To overcome this challenge, herein, we report the living cationic ring-opening polymerization of hetero Diels-Alder adducts. The scalable and modular synthesis of the cyclic monomers was achieved by a one-step protocol using readily available vinyl precursors. Subsequently, living polymerization of the cyclic monomers was examined, allowing the synthesis of vinyl polymers while controlling multiple factors, including molecular weight, dispersity, alternating sequence, head-to-head regioregularity, and end-group functionality. The living characteristics of the developed method were further demonstrated by block copolymerization. The synthesized vinyl polymers exhibited unique thermal properties and underwent fast photodegradation even under sunlight.

Abstract Sequence‐controlled semiconducting polymers represent a new frontier in organic electronics, where precise molecular sequence directly dictates device performance. However, achieving both high sequence fidelity and structural diversity remains a significant challenge using conventional synthetic protocols. To address this issue, we introduce a versatile halide‐pair‐driven multicomponent polymerization (MCP) strategy that enables the library synthesis of sequence‐controlled semiconducting poly(triarylamine)s (PTAAs). By optimizing halide pairing in conjunction with a rationally designed Buchwald ligand–Pd system featuring catalyst‐transfer capability, we achieved efficient sequential cascade aminations, thereby enabling the MCP. The versatility of this strategy was demonstrated through the synthesis of a library of sequence‐controlled PTAAs, including dendronized variants, underscoring its potential as a general platform for functional semiconducting material discovery.

To address the urgent need for CO 2 utilization in climate change mitigation, this study presents a highly efficient Zn-gallate catalyzed polymer synthesis, directly incorporating CO 2 alongside lactide and propylene oxide. This versatile catalyst facilitates both one-step random and sequential polymerization strategies, providing access to a diverse range of CO 2 -polymers. By precisely controlling composition and architecture, we synthesized random terpolymers, incorporating CO 2 , with catalytic activities of 1.7–3.6 kg/g-cat and 9.4 − 36 wt% PLA, and block copolymers involving CO 2 with catalytic activities of 0.7–3.0 kg/g-cat and 15 − 76 wt% PLA. These precisely tailored CO 2 -polymers display their potential to replace fossil-fuel-derived plastics like LDPE. • High performance CO 2 -polymer synthesis, tailored composition and architecture. • Zn-gallate (8.8 kg/g-Zn): 20 times better than previous heterogeneous Zn catalysts. • CO 2 -polymers surpass LDPE: potential sustainable fossil-fuel plastic replacement.

Since the discovery of single-atom catalysts (SACs) in 2011, research has primarily focused on achieving atomic dispersion, which can lead to their remarkable catalytic activity, selectivity, and atom utilization. In parallel, nanoparticles (NPs)-based catalysts have a long-standing history and a proven track record in electrocatalysis. Integration of single atoms (SAs) and NPs within a single catalytic framework has recently emerged as a promising strategy to enhance electrocatalytic performance beyond what each component can achieve on its own. Therefore, understanding these synergistic interactions is crucial for improving the activity, selectivity, and long-term stability of hybrid catalysts. Despite this potential, systematic investigations on these hybrid catalyst systems are relatively limited and present significant challenges. This review provides a comprehensive overview of the structural classifications, mechanistic insights, and recent advances in electrocatalytic applications of SA-NP hybrid systems. We further highlight synthetic strategies for nitrogen-doped carbon materials as supports that co-stabilize SAs and NPs, and critically discuss key challenges and future perspectives for the rational design and application of these advanced electrocatalysts are critically discussed.

Abstract The earth‐abundant II‐IV‐nitrides ZnSnN 2 and ZnGeN 2 are direct bandgap semiconductors with a wurtzite‐derived crystal structure. Their alloys, ZnSn x Ge 1 − x N 2 , have bandgaps tunable across the full visible spectrum, making them interesting for many optoelectronic applications. Here, electrical, structural, and optical properties of near‐stoichiometric ZnSn x Ge 1 − x N 2 alloys, i.e., where [Zn]/([Zn]+[Ge]+[Sn]) ≈ 0.5, are reported, for samples synthesized by reactive magnetron sputtering. These results reveal unprecedentedly high electrical mobilities in Ge‐rich alloys, with values of 136 and 400 cm 2 /Vs at room‐temperature and ≈100 K, respectively. The bandgaps are determined from optical absorption measurements combined with hybrid density functional calculations and reveal a significant Burstein–Moss shift in the Sn rich alloys. Finally, band alignments are determined in the sputter‐grown thin films by combining optical transmission measurements, hybrid density functional calculations, and UV photoelectron spectroscopy measurements, where the bandgap variation is predominantly caused by a shift of the conduction band edge. This work elucidates in unprecedented detail the tuning of optical and electrical properties in ZnSn x Ge 1 − x N 2 by variation of the chemical composition, where bandgap values of alloys with x ∈ [0.5−0.7] are suitable for top cell absorbers in two‐terminal tandem solar cells assuming a Si bottom cell.