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Conventional inorganic nanowire (NW) fibers are usually not stretchable and elastic, which may limit their practical applications. Inspired by the similarity between inorganic sub-1 nm NWs and polymer chains in dimension, and helical spring-like structure of cellulose in cherry bark, highly flexible and stretchable NW superlattice fibers composed of sub-1 nm GdOOH NWs are fabricated. The NW fibers could be twined, bent, twisted, and tied without any damage. When the strain is less than 10%, the fibers present elastic deformation. The elongation at break of the fibers usually reaches ≈40–50% and the highest elongation could reach ≈86%. Excellent flexibility and stretchability of the NW fibers are attributed to the well-aligned spring-like NWs assembled superlattice, which are demonstrated by scanning electron microscopy tests, synchrotron small-angle X-ray scattering, and obvious birefringence. Moreover, NW-nanoparticle (NP) fibers are fabricated, inspired by inorganic nanoparticle–reinforced polymers. The strength is improved compared with the NW fibers. Based on this work, it is possible to fabricate multifunctional, flexible, and stretchable inorganic NW materials composed of different inorganic sub-1 nm NWs, which may be useful in practical applications.

Membranes offer a potentially energy‐efficient and space‐saving solution to reduce CO2 emissions and combat global warming. However, engineering membranes with advanced materials for high permeance and reasonable selectivity is a pressing need. In this context, a series of carbazole‐based conjugated microporous polymer (CMP) membranes are fabricated with thicknesses of a few hundred nanometers through in situ electropolymerization for post‐combustion carbon capture. The findings reveal that various experimental conditions, including the monomer concentration, electric potential, and cyclic voltammetry (CV) cycling number, largely impact the polymerization degree of the carbazole‐based CMP, thus influencing the mode of polymer chain packing. An optimal polymerization degree leads to a larger micropore size and a higher fractional free volume (FFV), thus allowing fast CO2 transport. The study first demonstrates the feasibility of using CMPs to fabricate thin film composite (TFC) membranes for post‐combustion carbon capture and confirms the high controllability of their micropores. These insights provide instructive guidance for the future advancement of CMP applications in membrane fabrication for gas separation and other fields that require precise micropore generation and design. [ABSTRACT FROM AUTHOR]

External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h-1 at -1.1 V and CO Faradaic efficiency (FE) of 94.2% at -0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center.

Highly active and durable electrocatalysts are of great significance to accelerate the sluggish oxygen evolution and oxygen reduction reaction (OER and ORR) which are indispensable processes in practical devices such as metal–air batteries. Herein, the authors integrate morphological design with compositional manipulation, and successfully achieve well-defined CoNiFe sulfide mesoporous nanospheres (CoNiFe-S MNs). The as-prepared CoNiFe-S MNs exhibit superior OER and ORR catalytic activity, delivering a low overpotential of only 199 mV at a current density of 10 mA cm−2 in 1 m KOH solution and a half-wave potential of 0.78 V in 0.1 m KOH solution toward OER and ORR, respectively. The CoNiFe-S MNs involved Zn–air battery exhibits remarkable charge–discharge performance (voltage gap of 0.76 V at 2 mA cm−2) and high power density (over 140 mW cm−3). Extended-time durability tests validate the structural recoverability of the mesoporous morphology, and the remarkable performance can be attributed to the intrinsic synergistic effect of heterometallic ions. It is believed that the method could pave the way for the design of novel electrocatalysts for Zn–air batteries.

Construction of macro-materials with highly oriented microstructures and well-connected interfaces between building blocks is significant for a variety of applications. However, it is still challenging to confine the desired structures. Thus, well-defined building blocks would be crucial to address this issue. Herein, we present a facile process based on 1.8 nm Pd nanoclusters (NCs) to achieve centimeter-size assemblages with aligned honeycomb structures, where the diameter of a single tubular moiety is ∼4 μm. Layered and disordered porous assemblages were also obtained by modulating the temperature in this system. The reconciled interactions between the NCs were crucial to the assemblages. As a comparison, 14 nm Pd nanoparticles formed only aggregates. This work highlights the approach of confining the size of the building blocks in order to better control the assembly process and improve the stability of the structures. [Figure not available: see fulltext.].

Well-designed hybrid materials based on noble metal-free elements have great potential to generate hydrogen (H2 ) and oxygen (O2 ) sustainably via overall water splitting for developing practical energy-related technologies. Herein, an accessible method is presented to synthesize nickel diselenide (NiSe2 ) ultrathin nanowires decorated with amorphous nickel oxide nanoparticles (NiOx NPs) as multifunctional electrocatalysts (NSWANs) for hydrogen and oxygen evolution reaction (HER and OER). The NSWANs exhibit quite low HER and OER overpotentials of 174 and 295 mV, respectively, holding the current density of 20 mA cm-2 for 24 h continuous operations in alkaline media. Meanwhile, a cell voltage of 1.547 V at the current density of 10 mA cm-2 for overall water splitting has been achieved by the NSWANs for the practical application, which could maintain fascinating activity of 20 mA cm-2 for 72 h without degradation. The decorated NiOx NPs not only prevent the NiSe2 from further oxidation but also expose requisite active sites for electrocatalytic process. It is believed that this study may provide a valuable strategy to design high-efficiency electrocatalysts and expand the applications of selenide-based materials.

Highly active and robust eletcrocatalysts based on earth-abundant elements are desirable to generate hydrogen and oxygen as fuels from water sustainably to replace noble metal materials. Here we report an approach to synthesize porous hybrid nanostructures combining amorphous nickel-cobalt complexes with 1T phase molybdenum disulfide (MoS2) via hydrazine-induced phase transformation for water splitting. The hybrid nanostructures exhibit overpotentials of 70 mV for hydrogen evolution and 235 mV for oxygen evolution at 10 mA cm-2 with long-term stability, which have superior kinetics for hydrogen- and oxygen-evolution with Tafel slope values of 38.1 and 45.7 mV dec-1. Moreover, we achieve 10 mA cm-2 at a low voltage of 1.44 V for 48 h in basic media for overall water splitting. We propose that such performance is likely due to the complete transformation of MoS2 to metallic 1T phase, high porosity and stabilization effect of nickel-cobalt complexes on 1T phase MoS2.

Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these catalysts are likely to consist of a combination of single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained a challenging task. In this study, a model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom sites and CoMn dual‐atom sites on a nitrogen‐doped carbon substrate. By employing a combination of X‐ray adsorption spectroscopy and density functional theory calculations, the atomic configuration of Co/CoMn‐NC has been determined. Density functional theory calculations are also used to unequivocally identify Co‐atom within the CoMn dual‐atom motif as the predominate active site of the Co/CoMn‐NC model catalyst toward oxygen reduction reaction (ORR), which is further confirmed by in situ Raman spectroscopy. The cooperative interactions between Co single‐atom sites and CoMn dual‐atom sites can finely tune the d‐band center and ameliorate the adsorption and desorption behaviors of the intermediates, thereby facilitating ORR kinetic. Overall, the study introduces a systematic strategy to elucidate the structure and the superiority of the model system and provides new insights into atomically dispersed multi‐metal active sites, showcasing that enhanced catalytic performance extends beyond unified diatomic sites or monatomic sites. [ABSTRACT FROM AUTHOR]

Controlling the concentrations of H2O and CO2 at the reaction interface is crucial for achieving efficient electrochemical CO2 reduction. However, precise control of these variables during catalysis remains challenging, and the underlying mechanisms are not fully understood. Herein, guided by a multi-physics model, we demonstrate that tuning the local H2O/CO2 concentrations is achievable by thin polymer coatings on the catalyst surface. Beyond the often-explored hydrophobicity, polymer properties of gas permeability and water-uptake ability are even more critical for this purpose. With these insights, we achieve CO2 reduction on copper with Faradaic efficiency exceeding 87% towards multi-carbon products at a high current density of −2 A cm−2. Encouraging cathodic energy efficiency (>50%) is also observed at this high current density due to the substantially reduced cathodic potential. Additionally, we demonstrate stable CO2 reduction for over 150 h at practically relevant current densities owning to the robust reaction interface. Moreover, this strategy has been extended to membrane electrode assemblies and other catalysts for CO2 reduction. Our findings underscore the significance of fine-tuning the local H2O/CO2 balance for future CO2 reduction applications. While challenging, controlling H2O/CO2 concentrations at the reaction interface is critical for achieving efficient electrochemical CO2 reduction. This work demonstrates that polymer coatings on the catalyst surface can effectively tune local H2O/CO2 concentrations, leading to selective, energy efficient and robust CO2 electroreduction. [ABSTRACT FROM AUTHOR]

Objectives As a promising positron emission tomography (PET) tracer, [68Ga]Ga-fibroblast activation protein inhibitor-04([68Ga]Ga-FAPI-04) performs better than 2-[18F]fluoro-2-deoxy- d -glucose ([18F]FDG) at diagnosing primary and metastatic lesions in patients with various types of cancer. We investigated the utility of [68Ga]Ga-FAPI-04 PET/CT for the detection of primary and metastatic lesions in renal cell carcinoma (RCC). [18F]FDG PET/CT were used for comparison. Methods Twenty-two patients with suspected RCC or recurrent RCC were enrolled in our study. Among these patients, 14 were newly diagnosed with RCC, 3 had recurrent RCC, and 5 were excluded from further analysis due to having benign renal tumours. Seventeen patients with RCC underwent [68Ga]Ga-FAPI-04 PET/CT, and 6 of them also received [18F]FDG PET/CT. The positive detection rates were calculated and compared with those in patients who underwent both scans. Results Data from 17 patients with RCC (median age: 60.5 years, interquartile range [IQR]: 54-70 years) were evaluated. The positive detection rate of [68Ga]Ga-FAPI-04 PET/CT for RCC was 64.7% (11/17). Lymph node metastases (n = 44), lung metastasis (n = 1), and bone metastasis (n = 1) were detected. Six patients with RCC underwent [68Ga]Ga-FAPI-04 and [18F]FDG PET/CT. [68Ga]Ga-FAPI-04 PET/CT showed a higher positive detection rate than [18F]FDG PET/CT in detecting RCC (83.3% [5/6] vs. 50% [3/6], P  = 0.545). Additionally, [68Ga]Ga-FAPI-04 PET/CT has higher SUVmax (3.20 [IQR: 2.91-5.80 vs. 2.71 [IQR: 2.13-3.10], P  = 0.116) and tumour-to-background ratio (TBR) values (1.60 [IQR: 1.33-3.67] vs. 0.86 [0.48-1.21], P  = 0.028) than [18F]FDG PET/CT. Conclusions These findings suggest that [68Ga]Ga-FAPI-04 PET/CT has potential value in RCC diagnosis. Further studies are warranted to validate these results. Advances in knowledge Clinical utility of [68Ga]Ga-FAPI-04 in RCC remains unclear, and there are not many similar studies in the literature. We evaluated the role of [68Ga]Ga-FAPI-04 in diagnosing RCC. [ABSTRACT FROM AUTHOR]

Electrochemical CO2 reduction (CO2R) to valuable products provides a promising strategy to enable CO2 utilization sustainably. Here, we report the strategy of using Cu-DAT (3,5-diamino-1,2,4-triazole) as a catalyst precursor for efficient CO2 reduction, demonstrating over 80% selectivity towards multicarbon products at 400 mA cm−2, with intrinsic activity over 19 times higher than that of Cu nanoparticles. The catalyst's active phase is determined to be metallic copper wrapped with the DAT ligand. We attribute this enhanced CO2R performance to the accelerated steps of *CO adsorption and C–C coupling induced by the closely cooperated DAT ligand. [ABSTRACT FROM AUTHOR]

Electrocatalytic CO2 reduction (CO2R) coupled with renewable electricity has been considered as a promising route for the sustainability transition of energy and chemical industries. However, the unsatisfactory yield of desired products, particularly multicarbon (C2+) products, has hindered the implementation of this technology. This work describes a strategy to enhance the yield of C2+ product formation in CO2R by utilizing spatial confinement effects. The finite element simulation results suggest that increasing the number of shells in the catalyst wil lead to a high local concentration of *CO and promotes the formation of C2+ products. Inspired by this, Cu nanoparticles are synthesized with desired hollow multi‐shell structures. The CO2 reduction results confirm that as the number of shells increase, the hollow multi‐shell copper catalysts exhibit improved selectivity toward C2+ products. Specifically, the Cu catalyst with 4.4‐shell achieved a high selectivity of over 80% toward C2+ at a current density of 900 mA cm−2. Evidence from in situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy unveils that the multi‐shell Cu catalyst exhibits an enhanced *COatop coverage and the stronger interaction with *COatop compared to commercial Cu, confirming the simulation results. Overall, the work promises an effective approach for boosting CO2R selectivity toward value‐added chemicals. [ABSTRACT FROM AUTHOR]

Fe-based single-atom catalysts (SACs) have been recognized as attractive candidates for the oxygen reduction reaction (ORR). However, several limitations such as unsatisfactory intrinsic activity and poor stability hinder their practical applications, motivating further optimization of Fe-SACs which requires precise control of their composition and coordination environment. Herein, we establish a facile solvothermal method to incorporate Cu into Fe-SACs to form heterometallic SACs. We observe that the adjacent Cu atoms can regulate the coordination environment of FeN4 sites and significantly enhance the ORR activity. As a result, the heterometallic SACs show superior ORR catalytic performance compared to the mono-Fe-SAC counterpart (an enhancement factor of ∼5 times), delivering a half-wave potential (E1/2) of 0.889 V vs. RHE and a high kinetic current density (jk) of 4.77 mA cm−2 at 0.9 V vs. RHE, and also outperform the state-of-the-art Pt/C catalyst under identical testing conditions. [ABSTRACT FROM AUTHOR]

Harvesting solar energy for saline and polluted water purification is a sustainable and affordable solution to alleviate the stress on water shortages. However, the water evaporation rate relies on high optical intensity and suffers from inadequate energy conversion. Herein, a novel hybrid donor–acceptor dendritic nanosheets (denoted as DNS) composed of phosphomolybdic acid (PMA) clusters and porphyrin ligands is reported. Experimental results and molecular dynamics simulations indicate that the PMA and porphyrin are oriented attachment and assembled into a stable nanostructure. Benefiting from the advantages of the unique structure and photosensitive components, the DNS exhibits high evaporation rate of 2.23 kg m‐2 h‐1 with 90.9% energy efficiency under 1 sun irradiation. It is noteworthy that the evaporation performance is upgraded by innovative technology, and even under 0.5 sun that is close to the natural sunlight intensity, the evaporation rate reaches up to 1.31 kg m‐2 h‐1, which exceeds that of the vast majority of the reported evaporators. Furthermore, this evaporator also displays excellent seawater desalination and wastewater decontamination based on photo‐thermal distillation, highlighting its potential application toward water purification. [ABSTRACT FROM AUTHOR]

As a bridge between nanocrystal catalysts and single‐atom catalysts, single‐unit‐cell catalysts seem at first glance to be unavailable for catalysis due to quantum effects and synthetic difficulties. Here, 24 nm Cu9S5 nanowires are synthesized via the LaMer pathway. Interestingly, when polyoxometalate (POM) clusters are introduced during the nucleation process, the 0.9 nm Cu9S5 nanowires are finally formed via covalent co‐assembly, analog to A–B–A–B‐type block co‐polymerization in the polymer field ("A" and "B" represent Cu9S5 unit cells and POM clusters, respectively). Multiple characterizations show that Cu9S5 exists as single‐unit‐cell structure. Therefore, each unit cell can work as an isolated active site. The single‐unit‐cell structure exhibits higher electrocatalytic activity and Faradaic efficiency (FE) of formic acid (82.0% at −0.8 V vs reversible hydrogen electrode (RHE)) during CO2 electroreduction, while the nanocrystal structure generates HCOO−, methanol, and ethanol with low FEs. This study suggests that the single‐unit‐cell catalyst displays great potential for precise catalysis by the finite size effect. [ABSTRACT FROM AUTHOR]

2D catalysts combined with single atom sites are promising candidates to promote CO2 reduction performance, but the ability to target stable materials with distinct structure still remains challenging. Herein, a series of single metal atoms anchored 2D metal–organic framework nanosheets (MOF‐NS‐M) with visualized and well‐ordered mesoporous structures are fabricated and exhibit enhanced CO2 reduction activity and selectivity with the assistance of visible‐light. Encouragingly, the CO Faradaic efficiency of MOF‐NS‐Co exceeds 90% in a wide potential window of −0.5 to −1.0 V versus RHE and reaches 98.7% with 100 mV positive shift compared with the result measured under dark. The catalytic kinetics studies show a fast initial electron transfer to CO2 to form *COO−, thanks to the sufficient exposed active sites resulting from the nanosheet nature and adjusted electron transfer pathway caused by the porphyrin photoswitch. [ABSTRACT FROM AUTHOR]

Developing two‐dimensional (2D) and single atomic layered materials is a fascinating challenge. Here we successfully synthesize porphyrin‐based monoatomic layer (PML), a freestanding 2D porphyrin‐based material of monomer‐unit thickness (2.8 Å). The solvothermal method provides a bottom‐up approach for tailoring the monoatomic layer from the nanoscale to the milliscale. PMLs containing accurately tailorable M‐N4 units (M=Cu and Au) were synthesized, which present metal center‐dependent performance for CO2 electrocatalysis. PML with Cu‐N4 centers performs high faradaic efficiencies of HCOO− and CH4 (80.86 % and 11.51 % at −0.7 V, respectively) while PML with Au‐N4 centers generates HCOO− and CO as major products (40.90 % and 34.40 % at −0.8 V, respectively). Irreversible restructuring behavior of Cu sites is also observed. Based on the graphene‐like properties and metal center‐selectivity relationships, we believe that PML will play a distinct role in various applications. [ABSTRACT FROM AUTHOR]

Utilizing sustainable energy for chemical activation of small molecules, such as CO2, to produce important chemical feedstocks is highly desirable. The simultaneous production of CO/H2 mixture (syngas) from photoreduction of CO2 and H2O is highly promising. However, the relationships between structure, composition, crystallinity, and photocatalytic performance are still indistinct. Here, amorphous ultrathin CoO nanowires and polyoxometalate incorporated nanowires with even lower crystallinity were synthesized. The POM‐incorporated ultrathin nanowires exhibit high photocatalytic syngas production activity, reaching H2 and CO evolution rates of 11555 and 4165 μmol g−1 h−1 respectively. Further experiments indicate that the ultrathin morphology and incorporation of POM both contribute to the superior performance. Multiple characterizations reveal the enhanced charge–hole separation efficiency of the catalyst would facilitate the photocatalysis. [ABSTRACT FROM AUTHOR]

Utilizing sustainable energy for chemical activation of small molecules, such as CO2, to produce important chemical feedstocks is highly desirable. The simultaneous production of CO/H2 mixture (syngas) from photoreduction of CO2 and H2O is highly promising. However, the relationships between structure, composition, crystallinity, and photocatalytic performance are still indistinct. Here, amorphous ultrathin CoO nanowires and polyoxometalate incorporated nanowires with even lower crystallinity were synthesized. The POM‐incorporated ultrathin nanowires exhibit high photocatalytic syngas production activity, reaching H2 and CO evolution rates of 11555 and 4165 μmol g−1 h−1 respectively. Further experiments indicate that the ultrathin morphology and incorporation of POM both contribute to the superior performance. Multiple characterizations reveal the enhanced charge–hole separation efficiency of the catalyst would facilitate the photocatalysis. [ABSTRACT FROM AUTHOR]

Utilizing sustainable energy for chemical activation of small molecules, such as CO2, to produce important chemical feedstocks is highly desirable. The simultaneous production of CO/H2 mixture (syngas) from photoreduction of CO2 and H2O is highly promising. However, the relationships between structure, composition, crystallinity, and photocatalytic performance are still indistinct. Here, amorphous ultrathin CoO nanowires and polyoxometalate incorporated nanowires with even lower crystallinity were synthesized. The POM‐incorporated ultrathin nanowires exhibit high photocatalytic syngas production activity, reaching H2 and CO evolution rates of 11555 and 4165 μmol g−1 h−1 respectively. Further experiments indicate that the ultrathin morphology and incorporation of POM both contribute to the superior performance. Multiple characterizations reveal the enhanced charge–hole separation efficiency of the catalyst would facilitate the photocatalysis. [ABSTRACT FROM AUTHOR]

Utilizing sustainable energy for chemical activation of small molecules, such as CO2, to produce important chemical feedstocks is highly desirable. The simultaneous production of CO/H2 mixture (syngas) from photoreduction of CO2 and H2O is highly promising. However, the relationships between structure, composition, crystallinity, and photocatalytic performance are still indistinct. Here, amorphous ultrathin CoO nanowires and polyoxometalate incorporated nanowires with even lower crystallinity were synthesized. The POM‐incorporated ultrathin nanowires exhibit high photocatalytic syngas production activity, reaching H2 and CO evolution rates of 11555 and 4165 μmol g−1 h−1 respectively. Further experiments indicate that the ultrathin morphology and incorporation of POM both contribute to the superior performance. Multiple characterizations reveal the enhanced charge–hole separation efficiency of the catalyst would facilitate the photocatalysis. [ABSTRACT FROM AUTHOR]

Introduction: Extreme environments such as prolonged high temperatures and droughts can cause vulnerability of vegetation ecosystems. The dry-hot valleys of Southwestern China, known for their extremely high annual temperature, lack of water, and unique non-zonal "hot island" habitat in the global temperate zone, provide exceptional sites for studying how plant adapts to the prolonged dry and hot environment. However, the specific local biotic-environment relationships in these regions remain incompletely elucidated. The study aims to evaluate how valley-type Savanna vegetation species and their communities adapt to long-term drought and high-temperature stress environments., Methods: The study investigated the changes in species diversity and communities' aboveground biomass of a valley-type Savanna vegetation along an elevation gradient of Yuanmou dry-hot valley in Jinsha River basin, southwest China. Subsequently, a general linear model was utilized to simulate the distribution pattern of species diversities and their constituent biomass along the elevation gradient. Finally, the RDA and VPH mothed were used to evaluate the impacts and contributions of environmental factors or variables on the patterns., Results and Discussion: The field survey reveals an altitudinal gradient effect on the valley-type Savanna, with a dominant species of shrubs and herbs plants distribution below an elevation of 1700m, and a significant positive relationship between the SR , Shannon-Wiener , Simpson , and Pielou indices and altitudes. Relatively, the community aboveground biomass did not increase significantly with elevation, which was mainly due to a decreased biomass of herbaceous plants along the elevation. Different regulators of shrub-herbaceous plant species and their functional groups made different elevation patterns of species diversity and aboveground biomass in valley-type Savannas. Herbaceous plants are responsible for maintaining species diversity and ensuring stability in the aboveground biomass of the vegetation. However, the influence of shrubs on aboveground biomass became more pronounced as environmental conditions varied along the altitudinal gradient. Furthermore, species diversity was mainly influenced by soil and climatic environmental factors, whereas community biomass was mainly regulated by plant species or functional groups. The study demonstrates that the spatial pattern of valley-type Savanna was formed as a result of different environmental responses and the productive capacity of retained plant species or functional groups to climate-soil factors, highlighting the value of the Yuanmou dry-hot Valley as a microcosm for exploring the intricate interactions between vegetation evolution and changes in environmental factors., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2024 He, Shi, Fang, Shi, Wang, Yang, Yan, Yang, Yu, Liang, Zhao and Jiang.)

Electrochemical CO 2 reduction (CO 2 R) to valuable products provides a promising strategy to enable CO 2 utilization sustainably. Here, we report the strategy of using Cu-DAT (3,5-diamino-1,2,4-triazole) as a catalyst precursor for efficient CO 2 reduction, demonstrating over 80% selectivity towards multicarbon products at 400 mA cm -2 , with intrinsic activity over 19 times higher than that of Cu nanoparticles. The catalyst ' s active phase is determined to be metallic copper wrapped with the DAT ligand. We attribute this enhanced CO 2 R performance to the accelerated steps of *CO adsorption and C-C coupling induced by the closely cooperated DAT ligand.

Electrochemical CO 2 reduction provides a potential means for synthesizing value-added chemicals over the near equilibrium potential regime, i.e., formate production on Pd-based catalysts. However, the activity of Pd catalysts has been largely plagued by the potential-depended deactivation pathways (e.g., [Formula: see text]-PdH to [Formula: see text]-PdH phase transition, CO poisoning), limiting the formate production to a narrow potential window of 0 V to -0.25 V vs. reversible hydrogen electrode (RHE). Herein, we discovered that the Pd surface capped with polyvinylpyrrolidone (PVP) ligand exhibits effective resistance to the potential-depended deactivations and can catalyze formate production at a much extended potential window (beyond -0.7 V vs. RHE) with significantly improved activity (~14-times enhancement at -0.4 V vs. RHE) compared to that of the pristine Pd surface. Combined results from physical and electrochemical characterizations, kinetic analysis, and first-principle simulations suggest that the PVP capping ligand can effectively stabilize the high-valence-state Pd species (Pd δ+ ) resulted from the catalyst synthesis and pretreatments, and these Pd δ+  species are responsible for the inhibited phase transition from [Formula: see text]-PdH to [Formula: see text]-PdH, and the suppression of CO and H 2 formation. The present study confers a desired catalyst design principle, introducing positive charges into Pd-based electrocatalyst to enable efficient and stable CO 2 to formate conversion.

Five-axis laser scanning technology is an effective drilling method for special-shaped holes. Due to a gap in laser angle-of-incidence (AOI) control within a large scanning field, current technologies are challenging for fabricating large-size holes or special-shaped hole arrays. In this paper, a large scanning field five-axis laser concurrent drilling system was proposed. The laser AOI was independently controlled using two pairs of synchronous deflection mirrors. The laser control deviations under a large scanning field were investigated systematically by simulation and experiment. By establishing a complete correction method, the laser AOI control within a scanning field diameter of up to 35 mm was achieved. A series of special-shaped holes were fabricated concurrently on a 3.6 mm thick glass fiber reinforced plastic (GFRP), verifying that the AOI can be controlled by the five-axis laser scanning system. Our work provides a novel method to increase the scanning field of the five-axis laser scanning technology, expanding the application scope of the five-axis laser processing.

Inspired by the success of graphene, a series of single- or few-layer 2D materials have been developed and applied in the past decade. Here, the successful preparation of monolayer and bilayer 2D porphyrin-based metal-organic frameworks (MOFs) by a facile solvothermal method is reported. The structure transition from monolayer to bilayer drives distinct electronic properties and restructuring behaviors, which finally results in distinct catalytic pathways towards CO 2 electrocatalysis. The monolayer favors CO 2 -to-C 2 pathway due to the restructuring of CuO 4 sites, while CO and HCOO - are the major products over the bilayer. In photocoupled electrocatalysis, the Faradaic efficiency (FE) of the C 2 compounds shows a nearly fourfold increase on the monolayer than that under dark conditions (FE C2 increases from 11.9% to 41.1% at -1.4 V). For comparison, the light field plays a negligible effect on the bilayer. The light-induced selectivity optimization is investigated by experimental characterization and density functional theory (DFT) calculations. This work opens up a novel possibility to tune the selectivity of carbon products just by tailoring the layer number of the 2D material., (© 2022 Wiley-VCH GmbH.)

Developing efficient and robust heterogeneous metallophthalocyanine electrocatalysts for CO 2 reduction remains a challenge. Here, a general synthetic method of zinc-metallophthalocyanine (MPc) molecular layer/polyoxometalate (POM) sandwich lamellar material is developed, and thus improved performance of electrocatalytic and photocoupled electrocatalytic CO 2 reduction is achieved. The incorporation of POM could prevent the packing of MPc molecular layers from aggregation, which would be favorable to the exposure of active sites. The molecular layer sandwich catalyst presents superior CO 2 reduction activity, delivering the highest CO Faradaic efficiency (FE CO ) of 96.1% at -0.7 V vs RHE in dark field. Under light irradiation, over 93% FE CO is achieved in a broad potential range from -0.6 to -0.9 V vs RHE with a maximum of 96.2%, and the carbon monoxide turnover frequency could exceed 2060 h -1 . Photoelectrochemical tests and luminescence characterizations reveal the molecular layer is beneficial for carrier separation during light irradiation; density functional theory calculations and electron paramagnetic resonance indicated a 2-fold enhancement of the external light field on the catalytic performance.

Introducing an external light field can increase the intrinsic activity and energy efficiency for electrochemical CO 2 reduction. Herein, a synergistic strategy that introduces photosensitive components and visible light into a stable system is reported to improve the performance for CO 2 reduction. The catalytic kinetics studies indicate that the synergistic effect of implantation of cationic Ti and additional light driving is the primary responsibility for accelerating the first electron transfer to form a *COO - intermediate. This leads to a satisfactory CO 2 -to-CO conversion for Zr/Ti-NB-Co in terms of high selectivity (Faradaic efficiency of 93.6% at -0.7 V), remarkable catalytic activity (production rate up to 546 mmol g -1 h -1 at -1.1 V), excellent long-term stability (without performance decay over 11 h), and large turnover frequency of 1028 h -1 at -1.1 V under visible light. These results imply that the photodriven Ti-based porphyrin catalyst not only can deliver more electrons, but also can act as a photoswitch to adjust the electron transfer pathway., (© 2021 Wiley-VCH GmbH.)

2D catalysts combined with single atom sites are promising candidates to promote CO 2 reduction performance, but the ability to target stable materials with distinct structure still remains challenging. Herein, a series of single metal atoms anchored 2D metal-organic framework nanosheets (MOF-NS-M) with visualized and well-ordered mesoporous structures are fabricated and exhibit enhanced CO 2 reduction activity and selectivity with the assistance of visible-light. Encouragingly, the CO Faradaic efficiency of MOF-NS-Co exceeds 90% in a wide potential window of -0.5 to -1.0 V versus RHE and reaches 98.7% with 100 mV positive shift compared with the result measured under dark. The catalytic kinetics studies show a fast initial electron transfer to CO 2 to form *COO - , thanks to the sufficient exposed active sites resulting from the nanosheet nature and adjusted electron transfer pathway caused by the porphyrin photoswitch., (© 2020 Wiley-VCH GmbH.)

Developing two-dimensional (2D) and single atomic layered materials is a fascinating challenge. Here we successfully synthesize porphyrin-based monoatomic layer (PML), a freestanding 2D porphyrin-based material of monomer-unit thickness (2.8 Å). The solvothermal method provides a bottom-up approach for tailoring the monoatomic layer from the nanoscale to the milliscale. PMLs containing accurately tailorable M-N 4 units (M=Cu and Au) were synthesized, which present metal center-dependent performance for CO 2 electrocatalysis. PML with Cu-N 4 centers performs high faradaic efficiencies of HCOO - and CH 4 (80.86 % and 11.51 % at -0.7 V, respectively) while PML with Au-N 4 centers generates HCOO - and CO as major products (40.90 % and 34.40 % at -0.8 V, respectively). Irreversible restructuring behavior of Cu sites is also observed. Based on the graphene-like properties and metal center-selectivity relationships, we believe that PML will play a distinct role in various applications., (© 2020 Wiley-VCH GmbH.)

Utilizing sustainable energy for chemical activation of small molecules, such as CO 2 , to produce important chemical feedstocks is highly desirable. The simultaneous production of CO/H 2 mixture (syngas) from photoreduction of CO 2 and H 2 O is highly promising. However, the relationships between structure, composition, crystallinity, and photocatalytic performance are still indistinct. Here, amorphous ultrathin CoO nanowires and polyoxometalate incorporated nanowires with even lower crystallinity were synthesized. The POM-incorporated ultrathin nanowires exhibit high photocatalytic syngas production activity, reaching H 2 and CO evolution rates of 11555 and 4165 μmol g -1  h -1 respectively. Further experiments indicate that the ultrathin morphology and incorporation of POM both contribute to the superior performance. Multiple characterizations reveal the enhanced charge-hole separation efficiency of the catalyst would facilitate the photocatalysis., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)