A molecularly engineered MOF photocatalyst for CO production from visible light-driven CO2 reduction.

With the fast development of the social economy and the improvement of people's living standards, energy and environmental issues are attracting more and more attention. In the future, the great challenge for mankind is to shift energy supply from fossil energy to renewable energy. Solar energy is the most important renewable energy on Earth. However, low energy density and intermittency limit its practical application. Photocatalysis has broad application prospects in solar energy utilization. Photocatalysis can utilize solar energy to decompose water to produce hydrogen, reduce carbon dioxide to synthesize solar fuel, and degrade pollutants to purify the environment. However, the low photocatalytic efficiency limits its practical application. Thus, from the viewpoint of practical utilization, the improvement in methods and new photocatalysts are highly required. A total of 16 papers have been published in this issue, covering H2 production, CO2 reduction, H2O2 synthesis, and pollutant degradation. Among them, there are 10 papers about hydrogen production and 6 papers related to S-scheme heterojunction photocatalysts. We would like to express our sincere thanks to all the authors who submitted their interesting works to this special issue. A summary of all 18 accepted papers is provided as follows. Firstly, in article number 2200394, the authors present different functional ligands or metals incorporated into the parent metal-organic frameworks (MOFs) to enhance the photocatalytic performance of multivariate MOFs. The synthesis methods and unique advantages of multivariate MOFs-based photocatalysts are discussed. The recent advance in three multivariate MOFs for solar-to-chemical energy conversion are summarized according to mixed-metal MOFs, mixed-metal and mixed-ligand MOFs, and mixed-ligand MOFs. Finally, future perspectives and challenges in CO2 conversion and H2 evolution over Multivariate MOFs-based photocatalysts are discussed. In article number 2200364, Liu and colleagues reported enhanced CO2 photoreduction over Ni(OH)2-x/WO3 nanofibers, which were prepared by in situ growth of freestanding oxygen-vacancy Ni(OH)2-x nanosheets on WO3 nanofibers. The Ni(OH)2-x/WO3 nanofibers exhibit an enhanced CO production rate with respect to WO3 (54.4 vs 8.1 µmol g−1 h−1). The 13CO2 isotope tracing experiment confirmed that the CO product originated from the input CO2. The article with number 2200189 presents n-type CoP2 semiconductors as one of the main active components for efficient hydrogen evolution obtained from bulk P-CoV-LDH (layered double hydroxide). To achieve oriented control of carrier migration, the ZnxCd1−xS solid solution is effectively combined with P-CoV-LDH to synthesize a highly efficient and stable S-scheme heterojunction photocatalyst. The best P-CoV-LDH/ZnxCd1−xS 30% composite has a hydrogen evolution rate of 1244.3 µmol without noble metal additives, which is 6.4 times more than ZnxCd1−xS. Li and co-workers, in article number 2200143, reported g-C3N4 with edge grafting of 4-(1H-imidazol-2-yl) benzoic acid and NiS cocatalysts fabricated via a one-pot chemical condensation of monomers with urea and subsequent photodeposition. The obtained composites exhibit greatly enhanced visible-light photocatalytic performance for H2 evolution, in comparison with the undoped g-C3N4. The synergistic effect of bimetallic sulfide is discussed in article number 2200139, which reports the composite bimetallic sulfide ZnCo2S4 and CdS with excellent photocatalytic hydrogen evolution capability. The synergistic effect of zinc ions and cobalt ions enriches the redox-active sites, which provides favorable conditions for the photocatalytic hydrogen evolution reaction. The synergistic effect of bimetallic ions as the main driving force for the accelerated hydrogen precipitation reaction is analyzed by fluorescence and electrochemical characterization. The results of hydrogen production experiments show that the hydrogen evolution amount of ZnCo2S4/CdS is about 10 times that of single CdS. Article number 2200134 describes carbon nanotubes in situ grown onto g-C3N4 nanosheets via a chemical vapor deposition process, catalyzed by Au nanoparticles pre-deposited on g-C3N4 surface via deposition-precipitation. Systematic characterizations, in particular femtosecond transient absorption spectroscopy and time-resolved photoluminescence, prove that carbon nanotubes can efficiently extract the localized electrons in the tri-s-triazine units of g-C3N4, thereby enhancing charge carrier diffusion and separation. In article number 2200130, a donor–acceptor modified g-C3N4 conjugated copolymer is fabricated via facile thermal copolymerization of 2-aminobenzimidazole (abIM) and urea. The experimental results demonstrate that the abIM units are successfully incorporated into the framework of g-C3N4 and the main chemical structure of g-C3N4 is still preserved. These abIM units can serve as electron acceptors, extending the π-conjugated system and inducing the intramolecular charge transfer via an internal electric field. As a result, the construction of D–A structure not only improves the optical utilization efficiency but also facilitates the intramolecular migration of electrons and holes, leading to enhanced photocatalytic hydrogen evolution (2566 µmol g−1 h−1) as compared to pristine g-C3N4. Article number 2200113 presents a novel S-scheme heterojunction photocatalyst g-C3N4/PDA comprised of ultrathin g-C3N4 and polydopamine (PDA) constructed by in situ self-polymerization. The optimal photocatalyst presents an excellent H2O2 production rate of 3801.25 µmol g−1 h−1 under light irradiation, which is about 2 and 11 times higher than that of pure g-C3N4 and PDA, respectively, and exceeds most of the reported C3N4-based photocatalysts. The improvement of photocatalytic activity is ascribed to the synergistic effect of improved light absorption and promoted charge separation and transfer induced by the S-scheme heterojunction. In article number 2200030, a novel quaternary CdIn2S4-xSex solid-solution nanocrystal photocatalyst was prepared by one-step hydrothermal synthesis. The bandgap structure of CdIn2S4-xSex nanocrystals can be adjusted from 2.42 to 1.87 eV by varying the molar ratio of Se/S. Compared with pure CdIn2S4, the CdIn2S4-xSex solid-solution photocatalyst clearly represents excellent photocatalytic hydrogen production performance, while the CdIn2S4-xSex (x = 0.4) solid-solution nanocrystal exhibits the optimal hydrogen-production efficiency of 314.24 µmol h−1, which is 3.3 times superior to that of CdIn2S4 (94.83 µmol h−1). In article number 2200027, ZnS/TiO2 S-scheme heterojunction photocatalysts were constructed by in situ depositing ZnS nanoparticles on TiO2 nanofibers via hydrothermal method. A highly improved photocatalytic H2 evolution rate is achieved for the ZnS/TiO2 heterojunction as compared to the mono-component ZnS and TiO2. Remarkably, the TiO2/ZnS-5 sample possesses the highest H2 evolution rate of 5503.8 µmol g–1 h–1, which is 4.8 times of ZnS and 38.8 times of TiO2, respectively. In article number 2200009, highly dispersed Ni sites are planted on C3N5, an N-rich carbon nitride, by a facial two-step annealing method to construct a Ni-C3N5 material. The incorporation of Ni sites can significantly enhance the e–/h+ separation efficiency of C3N5 under light irradiation and promote the activation of O2 to produce reactive oxygen species. Compared with pristine C3N5 (with NO removal ratio of ≈35%), the as-prepared 0.1- or 0.25-Ni-C3N5 material can remove ≈54% continuous-flowing NO (initial concentration: 600 ppb) quickly in less than 25 min under white LED light irradiation. A novel sandwich-like hierarchical heterostructure of Ti3C2 MXene/WO3 is created by in situ growth of ultrathin WO3 nanosheets onto the surface of few-layer Ti3C2 nanosheets via a one-pot solvothermal synthesis strategy (article number 2100507). The resultant Ti3C2/WO3 heterostructure holds a large interface contact area, an intimate electronic interaction, and a short carrier migration distance, which is beneficial for bulk-to-surface and interfacial charge transfer. As expected, the as-prepared Ti3C2/WO3 nanohybrids exhibit superior visible-light-driven photoactivity and stability toward tetracycline hydrochloride decomposition. Article number 2100498 presents an S-scheme of Mn0.2Cd0.8S-diethylenetriamine/porous g-C3N4 heterojunction designed, which accelerates the charge transfer at the interface of Mn0.2Cd0.8S-diethylenetriamine and porous g-C3N4, and provides electrons for photocatalytic hydrogen production. Under the same light conditions, the hydrogen production efficiency of the composite is 11.42 mmol h–1 g–1, which is 30 times higher than that of porous g-C3N4. The paper "Porous Zn conformal coating on dendritic-like Ag with enhanced selectivity and stability for CO2 electroreduction to CO" (article number 2200374) presents uniform porous Zn conformal coating on high-curvature dendritic Ag nanoneedles by vacuum thermal evaporation. As the surface sacrificial shell, the dissolution and reconstruction of Zn protect the inner Ag core, thus enhancing the CO2 reduction stability of the composited samples. In article number 2200402, a step-scheme heterojunction consisting of thin TiO2 nanosheets and few-layered MoO3 structures is reported. With a decoration of a low dose of MoO3 layer by ball milling method, TiO2 shows a 3-fold increase in the hydrogen evolution rate. The presence of MoO3 promotes the electron-hole pair separation via the Step-scheme mechanism. Finally, in article number 2200381, a novel MOFs-derived In2O3/ZnO tubular S-scheme heterojunction photocatalyst for CO2 photoreduction is reported. Because of Fermi level difference and electron transfer, an internal electric field is produced at In2O3/ZnO heterojunction interfaces, which results in the formation of S-scheme heterojunctions. The CO2 photoreduction follows a *COOH-intermediate mechanism and the CO production rate (12.6 µmol g−1) with nearly 100% selectivity is obtained over In2O3/ZnO S-scheme photocatalyst. The authors declare no conflict of interest. Jiaguo Yu is a professor in the Faculty of Materials Science and Chemistry at the China University of Geosciences. He received his BS and MS degrees in chemistry from Central China Normal University and Xi'an Jiaotong University, respectively, and his PhD degree in materials science in 2000 from Wuhan University of Technology. In 2000, he became a Professor at Wuhan University of Technology. In 2021, he moved to the China University of Geosciences (Wuhan). His research interests include photocatalysis, adsorption, electrocatalysis and so on. He is a Foreign Member of Academia Europaea (2020), a Foreign Fellow of the European Academy of Sciences (2020), and a KIA Laureate of the 35th Khwarizmi International Award (2022). Kai Dai is a professor at the College of Physics and Electronic Information, Huaibei Normal University, Huaibei, China. He received Ph.D. degree from Shanghai University in 2007 and then worked as an assistant professor in Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences. He joined Huaibei Normal University in 2010 and his research interests mainly focus on semiconductor photocatalysis. Chuanbiao Bie obtained his Ph.D. degree in Materials Science and Engineering from Wuhan University of Technology (2021). He is now a postdoctoral researcher working in the Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences (Wuhan). His research interests are focused on semiconductor photocatalysis, including H2 evolution, CO2 reduction, H2O2 production, and organic synthesis.

The exploration of robust titanium-based metalorganic framework (MOF) photocatalysts for efficient CO 2 reduction is of critical significance but remains challenging. Herein, a hierarchically porous titanium-MOF (hMUV-10) anchored with ultrafine Pd nanoparticles was rationally designed via a convenient one-step in-situ water-etching strategy. The hierarchical MUV-10 structure provided abundant sites for the anchoring of Pd nanoparticles on the outside and inside of MOFs. The optimized Pd/hMUV-10 demonstrated an ultrahigh CO production rate of 65.9 mmol g −1 h −1 under light irradiation at 350°C, approximately two orders of magnitude higher than the state-of-the-art MOF-based catalysts and surpassed most reported inorganic semiconductor-based catalysts. The CO production rate under a relatively mild temperature of 200°C also reached as high as 3.36 mmol g −1 h −1 , and negligible activity decay was observed during continuous cycling measurement under 350°C. Theoretical calculations suggested that Pd enhanced CO 2 adsorption ability and reduced the energy barrier for CO 2 reduction, thereby leading to a highly improved CO yield from photothermal CO 2 reduction.

Synergistic effects of Cu7S4@Cu2O core-shell photocatalyst and S-scheme heterojunction in photocatalytic CO2 reduction

Novel honeycomb-like Ni-MOF enhanced hierarchical Bi2MoO6 microspheres for high efficient photocatalytic CO2 reduction

This study explores how the strategic material design introduced synergetic coupling of strong metal–support interaction (SMSI) between copper (Cu) nanoparticles and titanium dioxide (TiO2) loaded on dendritic fibrous nanosilica (DFNS), defects within TiO2, and localized surface plasmon resonance (LSPR) of Cu. Mechanistic insights were gained using in situ high-energy radiation fluorescence detection X-ray absorption near edge structure (HERFD-XANES) spectroscopy, electron microscopy, and finite-difference time-domain (FDTD) simulations. The introduction of copper nanoparticles onto the TiO2 surface induces a change in the electronic structure and surface chemistry of TiO2, due to the electronic interactions between Cu sites and TiO2 at the interface, inducing SMSI. This resulted in enhancing light absorption, efficient charge transfer, reducing electron–hole recombination and enhancing the overall catalytic efficiency. The activation energy for CO2 reduction was significantly reduced in light as compared to dark. Control experiments revealed a dominant role of photoexcited hot carriers, alongside photothermal effects, in driving CO2 reduction, supported by super-linear light intensity dependence and reduced activation energies. The unique interplay of O-vacancy defects, electron–hole separation in TiO2 and LSPR effects in Cu led to the excellent performance of the DFNS/TiO2–Cu10 catalyst. The catalyst outperformed the reported photocatalytic systems with a CO production rate of ∼3600 mmol gCu−1 h−1 (360 mmol gcat−1 h−1) with nearly 100% selectivity. A reaction mechanism was proposed based on the intermediates observed using the in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and co-related to the electron transfer pathways to different reactants using HERFD-XANES. The study concluded that the synergistic coupling of Cu LSPR, charge carrier separation via SMSI at the Cu–TiO2 interface, and O-vacancy defects stabilized by SMSI enhance the photocatalytic CO2 reduction performance of this hybrid system.

Emerging Nanomaterials for Light‐Driven Reactions: Past, Present, and Future

Reducing CO2 into fuels via photochemical reactions relies on highly efficient photocatalytic systems. Herein, we report a new and efficient photocatalytic system for CO2 reduction. Driven by electrostatic attraction, an anionic metal-organic framework Cu-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) as host and a cationic photosensitizer [Ru(phen)3]2+ (phen = 1,10-phenanthroline) as guest were self-assembled into a photocatalytic system Ru@Cu-HHTP, which showed high activity for photocatalytic CO2 reduction under laboratory light source (CO production rate of 130(5) mmol g-1 h-1, selectivity of 92.9%) or natural sunlight (CO production rate of 69.5 mmol g-1 h-1, selectivity of 91.3%), representing the remarkable photocatalytic CO2 reduction performance. More importantly, the photosensitizer [Ru(phen)3]2+ in Ru@Cu-HHTP is only about 1/500 in quantity reported in the literature. Theoretical calculations and control experiments suggested that the assembly of the catalysts and photosensitizers via electrostatic attraction interactions can provide a better charge transfer efficiency, resulting in high performance for photocatalytic CO2 reduction.

The incorporation of multiple functional groups or metal sites into predetermined positions of a metal–organic framework (MOF) cavity would obtain tailored MOF materials, which greatly facilitate their modulated light harvesting, band gap, and consequently photocatalytic activity. Herein, a multicomponent zirconium MOF, JLU-MOF58(Ni)-PDI, was achieved by incorporating PDI (short for perylene diimide) and Ni2+ sites into JLU-MOF58. JLU-MOF58(Ni)-PDI exhibited visible-light-driven reduction of CO2 in the absence of any additives under mild conditions. In addition, the CO production rate of JLU-MOF58(Ni)-PDI was 3.2 to 12.8 times higher than a series of classical materials, which can be assigned to the efficient introduction of the photosensitive fragments and catalytically active sites into the parent MOF. Furthermore, the catalytic mechanism was studied in detail by a series of experiments and density functional theory calculations.

Oxygen consumption and CO 2 , N 2 O, and N 2 production from a slurry of a slightly acidic soil incubated in a closed container with several different concentrations of NO ‐ 3 were investigated using a mass spectrometer. Under unshaken conditions, the rates of O 2 consumption and CO 2 production changed with time. Nitrous oxide and N 2 gases were produced even though there was ample O 2 in the atmosphere above the stagnant water. Under these conditions the rates of O 2 consumption and N 2 O, N 2 , and CO 2 production were controlled by the kind and rate of supply of electron acceptors to the sites of denitrification. When well shaken, the rate of O 2 consumption was constant. The CO 2 production rate had two distinctive values. The rate of CO 2 production when O 2 was still in the system was greater than the value obtained after O 2 in the system was all depleted. Nitrous oxide started to appear only when O 2 was completely consumed. Under the shaken conditions, the measured rates of O 2 consumption, CO 2 , and N 2 O production were independent of NO ‐ 3 concentration; however, the average life and the maximum concentration of N 2 O were directly related to initial NO ‐ 3 concentration. It is useful to define a parameter, denitrification intensity (DNI), which is proportional to the potential maximum rate of electron production for a soil with constant microbial activity under fixed temperature. Determination of the DNI must be made when the rate of electron acceptor (NO ‐ 3 or NO ‐ 2 ) supply is not limiting the reaction. Under these conditions, the inhibition of conversion of N 2 O to N 2 results in the rate of N 2 O‐N production which is greater than the rate of production of the sum of N 2 O‐N and N 2 ‐N without inhibition. If the rate of supply of electron acceptors (NO ‐ 3 or NO ‐ 2 ) is smaller than DNI, a parameter, gaseous nitrogen production rate (GNPR), the magnitude of which is unaffected by the inhibition of conversion of N 2 O to N 2 , characterizes the denitrification process.

This study has designed and implemented a library of hetero‐nanostructured catalysts, denoted as Pd@Nb2O5, comprised of size‐controlled Pd nanocrystals interfaced with Nb2O5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb2O5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH4 production rates as high as 0.75 and 0.11 mol h−1 gPd −1, respectively. By contrast, using small Pd nanocrystals, a CO production rate surpassing 18.8 mol h−1 gPd −1 is observed with 99.5% CO selectivity. These performance metrics establish a new milestone in the champion league of catalytic nanomaterials that can enable solar‐powered gas‐phase heterogeneous CO2 reduction. The remarkable control over the catalytic performance of Pd@Nb2O5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.

In this work, we have designed and synthesized nickel-laden dendritic plasmonic colloidosomes of Au (black gold-Ni). The photocatalytic CO2 hydrogenation activities of black gold-Ni increased dramatically to the extent that measurable photoactivity was only observed with the black gold-Ni catalyst, with a very high photocatalytic CO production rate (2464 ± 40 mmol gNi-1 h-1) and 95% selectivity. Notably, the reaction was carried out in a flow reactor at low temperature and atmospheric pressure without external heating. The catalyst was stable for at least 100 h. Ultrafast transient absorption spectroscopy studies indicated indirect hot-electron transfer from the black gold to Ni in less than 100 fs, corroborated by a reduction in Au-plasmon electron-phonon lifetime and a bleach signal associated with Ni d-band filling. Photocatalytic reaction rates on excited black gold-Ni showed a superlinear power law dependence on the light intensity, with a power law exponent of 5.6, while photocatalytic quantum efficiencies increased with an increase in light intensity and reaction temperature, which indicated the hot-electron-mediated mechanism. The kinetic isotope effect (KIE) in light (1.91) was higher than that in the dark (∼1), which further indicated the electron-driven plasmonic CO2 hydrogenation. Black gold-Ni catalyzed CO2 hydrogenation in the presence of an electron-accepting molecule, methyl-p-benzoquinone, reduced the CO production rate, asserting the hot-electron-mediated mechanism. Operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) showed that CO2 hydrogenation took place by a direct dissociation path via linearly bonded Ni-CO intermediates. The outstanding catalytic performance of black gold-Ni may provide a way to develop plasmonic catalysts for CO2 reduction and other catalytic processes using black gold.

Due to land use intensification and drainage many peatlands have lost their C sink function. Consequently, rewetting has become an important strategy to mitigate increased greenhouse gas emissions from degraded peatlands. Whereas CO2 emissions decrease under reducing conditions upon waterlogging, CH4 production rates increase. The exact effect of rewetting may depend on the initial degree of degradation of a peatland and resulting peat quality. Therefore, the aim of this study was to elucidate waterlogging effects on C mineralization rates of peat from two contrasting sites. Near-surface peat soils from a long-term drained area and a rewetted site with newly formed floating mat were incubated under aerobic and anaerobic conditions for 90 days. CO2 and CH4 production rates were measured with weekly intervals. At the beginning and at the end of the incubation, liquid phase samples were taken and analysed for (in)organic ions, element stoichiometry, UV absorbance spectra and, DOC concentrations. When CO2 and CH4 production had reached steady states, we measured C-, N- and P-related hydrolytic enzyme activities of the peat. We expected that hydrolytic enzyme activities decrease, resulting in lower CO2 production rates, under anaerobic conditions. Furthermore, it was hypothesized that C mineralization rates of the pristine floating mat would exceed those of the degraded drained peatland due to higher availability of more labile organic matter in the former site. As expected, rewetting, as simulated by anoxic incubations, slowed CO2 production rates and activities of beta-glucosidase as compared to the oxic controls. Moreover, the availability of oxygen stimulated near-surface peat decomposition supported by a strong decrease in DOC concentrations after aerobic incubation in the degraded peat. However, the average rate of CO2 production was six times higher in the degraded drained site compared to the restored floating mat (189.84 and 29.76 μmol CO2 g dw-1 d-1, respectively). CH4 production from the long-term drained site began after 75 days of anoxic incubation and was almost negligible compared to the restored site (0.06 v. 0.46 g dw-1 d-1 after 75 days of incubation, respectively). Due to the high CO2 production rates measured at the drained site, it is unlikely that high peat recalcitrance was the cause of low CH4 production. In contrast to CO2 production rates, there were no significant differences in beta-glucosidase activities between the two sites. Probably other substrates than cellulose were involved in peat decomposition from the degraded site compared to decomposition of the floating mat. Therefore, this may either imply that degraded peat has an adapted community of microbes releasing enzymes that are able to breakdown a wide spectrum of organic sources, including aromatics. Or, alternatively, the build-up of phenolics in the Sphagnum-rich restored site inhibits hydrolytic enzyme activity and consequently leads to lower CO2 production rates. Thus, under anoxic conditions, overall low activities of hydrolytic enzymes partly supported the enzymatic latch paradigm. We have shown that rewetting slows CO2 production rates and may not result in immediate CH4 production. Moreover, peat quality and enzyme activities appear an important control on peatland restoration that requires further investigation.

One-pot solvothermal synthesis of In-doped amino-functionalized UiO-66 Zr-MOFs with enhanced ligand-to-metal charge transfer for efficient visible-light-driven CO2 reduction

Photocatalysis is known as a new and cost-effective method to solve the problems of energy shortage and environmental pollution. Although the application of this method seems practical, finding an efficient and stable photocatalyst with a suitable bandgap and visible-light sensitivity remains challenging. In this context, vanadate compounds photocatalysts have been synthesized and used as emerging composites, and their efficiency has been improved through elemental doping and morphology modifications. In this review, the major synthesis methods, and the design of the latest photocatalytic compounds based on vanadate are presented. In addition, the effect of vanadate microstructures on various photocatalytic applications such as hydrogen production, CO2 reduction, and removal of organic pollutants and heavy metals are discussed. For instance, the application of a 2D-1D BiVO4/CdS heterostructure photocatalyst enhances 40 times the hydrogen production from benzyl alcohol than pure BiVO4. Similarly, the InVO4/Bi2WO6 composite has a superior photocatalytic capability for the reduction of CO2 into CO compared to pure InVO4. A CO production rate of 18 μmol.g−1.h−1 can be achieved by using this heterostructure. Regarding the organic pollutants’ removal, the use of Montmorillonite/BiVO4 structure allows a complete removal of Brilliant Red 80 dye after only 2 hours of irradiation. Finally, copper heavy metal is reduced to 90 % in water, by using BiVO4/rGO/g-C3N4 optimized photocatalyst structure. Other examples on decorated vanadate compounds for enhancing photocatalytic activities are also treated.

Electroreduction of CO2 to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO2 utilization. Herein, we report a hierarchical CuS h...